Title of Invention

COVER COATING COMPOSITION FOR GLASS LINING

Abstract Provided is a cover coating composition for a glass lining comprising a frit constituting the composition which mainly includes 65 to 75 mol% of Si02, 2 to 8 mol% of Zr02, 10 to 22 mol% of R20 where R represents Li, K, or Cs, and 2 to 12 mol% of R"O where R" represents Mg, Ca, Sr, or Ba, and the frit is free of Na20, and said cover coating composition for a glass lining may further contain a metal fiber.
Full Text DESCRIPTION
RARE EAETH METAL COMPLEX. CATALYST FOR POLYMERIZATION AND PROCESS FOR PRODUCING POLYMER
FIELD OF THE INVENTION
[0001] The present invention relates to a rare earth metal complex and a process for producing the same, a catalyst for olefin or lactone polymerization containing the rate earth metal complex, as well as a process for producing a polymer of an olefin or of a polar monomer such as a lactone.
BACKGROUND ART
[0002] A metallocene complex having one cyclopentadiene ligand is a compound which is called a half metallocene complex and utilized as a catalytic component for polymerizing various olefins, and it is known that the property thereof (a catalytic activity on a polymerization reaction) greatly varies depending on the kind of its central metal. Inter alia, it is known that a polymerization catalytic component comprising a half metallocene complex having a Group 3 metal or a lanthanoid metal (hereinafter, a Group 3 metal and a lanthanoid metal are collectively referred to as rare earth metals) as a central metal can be used in the polymerization or copolymerization of ethylene and cr olefins, the polymerization or copolymerization of aromatic olefin monomers such as styrene, and the polymerization or copolymerization of cyclic olefin monomers such as norbornene (see WO 2006/004068). It is also known that such a half metallocene complex having a rare earth metal as a central metal can be used in the polymerization of cyclohexene oxide, and the copolymerization of cyclohexene oxide and carbon dioxide (see

Macromolecules 2005, 38, 4089). It is known that a half metallocene complex having lanthanum as a central metal can be used in the syndiotactic polymerization of a methacrylate ester, the block copolymerization of ethylene and a methacrylate ester, the polymerization of isocyanide. and the polymerization of acrylonitrile (see J. Polym. Sci.: Part A: Polym. Chem. 2001, 39, 1382). Thus, the half metallocene complex having a rare earth metal as a central metal is a useful metal complex for which many utilities are expected. On the other hand, as a metal complex having a ligand in which a cyclopentadiene derivative and a phenol derivative are linked with a Group 14 atom, a Group 4 transition metal complex is known as a catalyst for olefin polymerization (see JP-A-09-87313), but no rare earth metal complex is known.
[0003] The polymers of lactone compounds such as e~caprolactone which can be industrially produced at low cost are useful as modifiers for polyurethane, coating resins and plastics. Among those polymers, particularly the lactone polymer with a high molecular weight attracts attention as a biodegradable polymer. As a process for producing the high-molecular weight polymer of a lactone, a method of ring-opening polymerization of a lactone using a rare earth alkoxide as a catalyst (see WO 91/05001), or a method of ring-opening polymerization of a lactone using a rare earth complex having a cyclopentadiene ligand as a catalyst is known (see JPA-05-247184). After that, regarding the ring-opening polymerization of a lactone using a rare earth complex as a catalyst, efforts for efficiently obtaining a polymer having a narrow molecular weight distribution have been reported (see Macromolecules 1999, 29, 1798).
SUMMARY OF THE INVENTION Problems to be Solved by the Invention

[0004] The first object of the present invention is to provide a novel rare earth metal complex which can be utilized as a catalytic component for polymerizing an olefin or a polar monomer such as a lactone, and a process for producing the same.
The second object of the present invention is to provide a process for producing a polymer or a copolymer of an olefin using such a catalytic component comprising a rare earth metal complex.
The third object of the present invention is to provide a process for producing a polymer of a polar monomer using such a catalytic component comprising a rare earth metal complex, inter aha, a process for efficiently producing a high-molecular weight polymer of a lactone.
Means for Solving the Problems
[0005] According to the first aspect, the present invention provides a rare
earth metal complex represented by the formula (l)-

wherein
A represents a Group 14 element of the periodic table,
Cp represents a group having a substituted or unsubstituted cyclopentadienyl anion moiety,
Ln represents a Group 3 metal atom or a lanthanoid metal atom.
R1. R2. R3, R4, R°, and Re are the same or different, and represent a hydrogen atom, a halogen atom, an alkyl group having 1 to 20 carbon atoms.

an aryl group having 6 to 20 carbon atoms, an aralkyl group having 7 to 20 carbon atoms, a silyl group substituted with a hydrocarbon group having 1 to 20 carbon atoms, an alkoxy group having 1 to 20 carbon atoms, an aryloxy group having 6 to 20 carbon atoms, an aralkyloxy group having 7 to 20 carbon atoms, or an amino group substituted with a hydrocarbon group having 1 to 20 carbon atoms,
R7 represents an alkyl group having 1 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, or an aralkyl group having 7 to 20 carbon atoms,
provided that, in R1 to R7, the alkyl group, the aryl group, the aralkyl group, the alkoxy group, the aryloxy group, the aralkyloxy group or the hydrocarbon group may be substituted with a halogen atom,
R1 and R2 may be bonded together to form a ring,
the adjacent groups of R3, R4, R5 and R6 may optionally be bonded together to form a ring, respectively,
m Xs are the same or different, and represent a monoanionic Iigand,
n Ys are the same or different, and represent a neutral Iigand,
m represents an integer of 1 to 3, and
n represents an integer of 0 to 3. [0006] According to the second aspect, the present invention provides a process for producing a rare earth metal complex represented by the formula (l) comprising the step of reacting a substituted or unsubstituted cyclopentadiene compound represented by the formula (2):


(2)

wherein A, Cp, R1, R2, R3, R4, R5, RG and R7 are the same as defined above with a rare earth metal compound represented by the formula (3):
R8-Lnrf
wherein Ln, X, Y, m and n are the same as defined above, and R8 represents
an alkyl group optionally substituted with a silyl group substituted with a
hydrocarbon group having 1 to 20 carbon atoms, or an aralkyl group
optionally substituted with an amino group substituted with a hydrocarbon
group having 1 to 20 carbon atoms.
[0007] According to the third aspect, the present invention provides a
catalytic component for olefin polymerization containing the rare earth
metal complex represented by the formula (l).
[0008] According to the fourth aspect, the present invention provides a
catalyst for olefin polymerization, obtained by contacting the catalytic
component for olefin polymerization with at least one compound selected
from the group consisting of the following aluminum compounds (Al) to (A3)
and the following boron compounds (Bl) to 033):
Aluminum compounds (A):
(Al): an organoaluminum compound represented by the formula:
(E0-A1Z (3-Hi; (A2): a cyclic aluminoxane having a structure represented by the formula:
{-Al(E2)-0-}b; and (A3): a linear aluminoxane having a structure represented by the formula:
E3{-Al(E3)-0-UKER)2 wherein a represents a number satisfying 0
plural E2s and plural E3s may be the same or different, Z represents a hydrogen atom or a halogen atom, and plural Zs may he the same or different! and Boron compounds (B):
(Bl)- a boron compound represented by the formula1 BQ1Q2Q3;
(B2): a boron compound represented by the formula:
GHBQLQSQ^)-; and (B3): a boron compound represented by the formula:
(L'-HMBQiQ^Q*)" wherein B represents a boron atom in the trivalent state, Q1, Q2, Q3 and Q4 each represent independently a halogen atom, a hydrocarbon group, a halogenated hydrocarbon group, a substituted silyl group, an aBcoxy group or a disubstituted amino group, G+ represents an inorganic or organic cation, and L1 represents a neutral Lewis base.
[0009] According to the fifth aspect, the present invention provides a process for producing an olefin polymer comprising the step of polymerizing an olefin in the presence of the catalyst for olefin polymerization. [0010] According to the sixth aspect, the present invention provides a process for producing a polymer of a polar monomer comprising the step of contacting a polar monomer with the rare earth metal complex represented by the formula (l) to polymerize the monomer.
[0011] According to the seventh aspect, the present invention provides a process for producing a polymer of lactones comprising the step of contacting a lactone with the rare earth metal complex represented by the formula (l) to ring-opening polymerizing the lactones.
[0012] According to the eighth aspect, the present invention provides a process for producing a polymer of an alkylene oxide comprising the step of

contacting an alkylene oxide with the rare earth metal complex represented by the formula (l) to ring-opening polymerize the alkylene oxides. [0013] According to the ninth aspect, the present invention provides a process for producing an acrylate ester polymer or a methacrylate ester polymer comprising the step of contacting an acrylate ester or a methacrylate ester with the rare earth metal complex represented by the formula (l) to polymerize the ester.
EFFECTS OF THE INVENTION
[0014] The novel rare earth metal complex of the present invention is useful, for example, as a catalyst for the polymerization reaction of an olefin. In addition, the use of the rare earth metal complex of the present invention as a catalyst makes it possible to polymerize a polar monomer and enables the production of, for example, a lactone polymer having a high molecular weight at a good yield at a relatively low temperature in a short time.
BEST EMBODIMENTS FOR CARRYING OUT THE INVENTION [0015] Examples of the group having a cyclopentadienyl anion moiety represented by Cp in the rare earth metal complex of the formula (l) (hereinafter, abbreviated as a rare earth metal complex (l)) include a cyclopentadienyl group, an indenyl group, and a fluorenyl group, each of which may be substituted or unsubstituted.
Specific examples of the group having a cyclopentadienyl anion moiety include substituted or unsubstituted cyclopentadienyl groups such as a cyclopentadienyl group, a methylcycl op entadienyl group, a dimethylcyclopentadienyl group, a trimethylcyclopentadienyl group, a tetramethylcyclopentadieny] group, an ethylcyclopentadienyl group, a n-propylcycl op entadienyl group, an isoprop ylcycl op entadienyl group, a

n-butylcyclopentadienyl group, a sec-butylcyclopentadienyl group, a tert-butylcyclopentadienyl group, a tetrahydroindenyl group, an octahydxofluorenyl group, a phen ylcycl op entadi enyl group, a trimethylsilylcyclopentadienyl group, and a
tert-butyl dimethylsily ley el op entadi enyl group; substituted or unsubstituted indenyl groups such as an indenyl group, a methylindenyl group, a dimethylindenyl group, an ethylindenyl group, a n-propylindenyl group, an isopropylindenyl group, a n-butylindenyl group, a sec-butylindenyl group, a tert-butylindenyl group, and a phenylindenyl group; and a fluorenyl group, and substituted fluorenyl groups such as a 2-methylfluorenyl group, a 2,7'dimethylfluorenyl group, a 2-ethylfluorenyl group, a 2,7-diethylfluorenyl group, a 2-n-propylfluorenyl group, a 2,7di-n-propylfluorenyl group, a 2-isopropylfluorenyl group, a 2,7-diisopropylfluorenyl group, a 2-n-butylfl.uorenyl group, a 2-sec-butylfluorenyl group, a 2-tert-butylfIuorenyl group, a 2,7-drn-butylfluorenyl group, a 2,7-di-sec-butylfluorenyl group, a 2,7-di-tert-butyLfluorenyl group, a 3,6-di-tert'butylfIuorenyl group, a 2-phenyLSuorenyl group, a 2,7-di-phenylfluorenyl group, and a 2-methylphenylfluorenyl group, and preferably a cyclopentadienyl group, a methylcyclopentadienyl group, a dimethylcyclopentadienyl group, a trimethylcyclopentadienyl group, a tetramethylcyclopentadienyl group, and a tert-butylcyclopentadienyl group. [0016] In the rare earth metal complex (l) and the substituted or unsubstituted cyclopentadiene compound represented by the formula (2) (hereinafter, abbreviated as a cyclopentadiene compound (2)), examples of the Group 14 element of the periodic table represented by A include a carbon atom, a silicon atom, and a germanium atom, and preferably a carbon atom and a silicon atom. [0017] In substituents R1, R2. R3, R4. R5 and R6. examples of the halogen

atom include a fluorine atom, a chlorine atom, a bromine atom, and an iodine atom, and preferably a chlorine atom.
[0018] InsubstituentsR1,^, R3,R4,R5, Re and R7, specific examples of the alkyl group having 1 to 20 carbon atoms include a methyl group, an ethyl group, a n-propyl group, an isopropyl group, a n-butyl group, a sec-butyl group, a tert-butyl group, a n-pentyl group, a neopentyl group, an amyl group, a n-hexyl group, a heptyl group, a n-octyl group, a n-nonyl group, a n-decyl group, a n-dodecyl group, a n-tridecyl group, a tetradecyl group, a pentadecyl group, a hexadecyl group, a heptadecyl group, an octadecyl group, a nonadecyl group, and a n-eicosyl group, and preferably a methyl group, an ethyl group, an isopropyl group, a tert-butyl group, an amyl group, and the like.
In substituents R1, R2, R3, R4, R5, R6 and R7, specific examples of the halogen-substituted alkyl group having 1 to 20 carbon atoms include the above alkyl groups which are substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom or an iodine atom. [0019] In substituents R', R2, R3, R4, RB, Rs and R7, specific examples of the aryl group having 6 to 20 carbon atoms include a phenyl group, a 2-tolyl group, a 3-tolyl group, a 4- tolyl group, a 2,3-xylyl group, a 2,4-xylyl group, a 2,5-xylyl group, a 2,6-xylyl group, a 3,4-xylyl group, a 3,5-xylyl group, a 2,3,4-trimethylphenyl group, a 2,3,5-trimethylphenyl group, a 2,3,6-trimethylphenyl group, a 2,4,6-trimethylphenyl group, a 3,4,5-trimethylphenyl group, a 2,3,4,5-tetramethylphenyl group, a 2,3,4,6-tetramethylphenyl group, a 2,3,5,6'tetramethylphenyl group, a pentamethylphenvl group, an ethylphenyl group, a n-propylphenyl group, an isopropylphenyl group, a n-butylphenyl group, a sec-butylphenyl group, a tert-butylphenyl group, a n-pentylphenyl group, a neopentylphenyl group, a n-hexylphenyl group, a n-octylphenyl group, a n-decylphenyl group, a

n-dodecylphenyl group, a n-tetradecylphenyl group, a naphthyl group, and an anthracenyl group, and preferably a phenyl group.
In substituents R1, R3, R3, RA, R5. Rfi and R\ specific examples of the aryl group having 6 to 20 carbon atoms substituted with a halogen include the above aryl groups which are substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom or an iodine atom. [0020] In substituents R1, R2, R3, R4, R5, R6 and R7, specific examples of the aralkyl group having 7 to 20 carbon atoms include a benzyl group, a (2-methylphenyDmethyl group, a (3-methylphenyl)methyl group, a (4-methylphenyl)methyl group, a (2,3-dimethylphenyDmethyl group, a (2,4"dimethylphenyl)methyl group, a (2,5-dimethylphenyl)methyl group, a (2,6-dimethyrphenyl)methyl group, a (3,4-dimethylphenyl)methyl group, a (4,6-dimethylphenyl)methyl group, a (2,3,4-trimethylphenyl)methyl group, a (2.3,5trimethylphenyl)methyl group, a (2,3,6-trimethylphenyl)methyl group, a (3,4,5-trimethylphenyl)methyl group, a (2,4,6-trimethylphenyl)methyl group, a (2,3,4,5-tetramethylphenyl)methyl group, a (2,3,4,6-tetramethylphenyDmethyl group, a
(2,3,5,6-tetramethylphenyDmethyl group, a (pentamethylphenyl)methyl group, an (ethylphenyl)methyl group, a (n-propyrphenyl)methyl group, an (isopr op yip henyDm ethyl group, a (nbutylphenyDmethyl group, a (sec-butylphenyl)methyl group, a (tert'butylphenyl)methyl group, a (n-pentylphenyl)methyl group, a (neopentylphenyl)methyl group, a (n-hexylphenyl)methyl group, a (n-octylphenyl)methyl group, a (n-decylphenyDmethyl group, a (n-decylphenyl)methyl group, a naphthylmethyl group, and an anthracenylmethyl group, and preferably a benzyl group.
In substituents R!; R2, R3, R4, R5, R^ and R7, specific examples of the aralkyl group having 7 to 20 carbon atoms substituted with a halogen

include the above aralkyl groups which are substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom or an iodine atom. [0021] In substituents R1. R2, R3, R4, R5, and R6, examples of the hydrocarbon group of the silyl group substituted with the hydrocarbon group include alkyl groups each having 1 to 10 carbon atoms such as a methyl group, an ethyl group, a n-propyl group, an isopropyl group, a n-butyl group, a sec-butyl group, a tert-butyl group, an isobutyl group, a n-pentyl group, a nhexyl group, a cyclohexyl group, a n-heptyl group, a n-octyl group, a n-nonyl group, and a n-decyl group, and aryl groups such as a phenyl group. Specific examples of such a silyl group substituted with hydrocarbon having 1 to 20 carbon atoms include monosubstituted silyl groups having 1 to 20 carbon atoms such as a methylsilyl group, an ethylsilyl group, and a phenylsilyl group, disubstituted silyl groups substituted with hydrocarbon groups each having 1 to 20 carbon atoms such as a dimethylsilyl group, a diethylsilyl group, and a diphenylsilyl group, and trisubstituted silyl groups substituted with a hydrocarbon group having 1 to 20 carbon atoms such as a trimethylsilyl group, a triethylsilyl group, a tri-n-propylsilyl group, a triisopropylsilyl group, a tri-n-butylsilyl group, a tri-sec-butylsilyl group, a tri-tert-butylsilyl group, a trrisobutylsilyl group, a tert-butyl-dimethylsilyl group, a tri-n-pentylsilyl group, a tri-n-hexylsilyl group, a tricyclohexylsilyl group, and a triphenylsilyl group, and preferably a trimethylsilyl group, a tert-butyl dimethylsilyl group, and a triphenylsilyl group.
Besides the above-described hydrocarbon groups, examples of the hydrocarbon group constituting a substituted silyl group include hydrocarbon groups substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom, or an iodine atom. [0022] In substituents R1, R2, R3, R4, R5, andRs, specific examples of the alkoxy group having 1 to 20 carbon atoms include a methoxy group, an

ethoxy group, a n-propoxy group, an isopropoxy group, a n-butoxy group, a sec-butoxy group, a tert-butoxy group, a n-pentyloxy group, a neopentyloxy group, a n-hexyloxy group, a iroctyloxy group, a n-nonyloxy group, a n-decyloxy group, a n-dodecyloxy group, a n-undecyloxy group, a n-dodecyloxy group, a tridecyloxy group, a tetradecyloxy group, a n-pentadecyloxy group, a hexadecyloxy group, a heptadecyloxy group, an octadecyloxy group, a nonadecyloxy group, and a n-eicosyloxy group, and preferably a methoxy group, an ethoxy group, and a tert-butoxy group.
Specific examples of the alkoxy group having 1 to 20 carbon atoms substituted with a halogen include the abvove alkoxy groups which are substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom or an iodine atom.
[0023] In substituents R1, R2, R3, R*. R5, and R6, specific examples of the aryloxy group having 6 to 20 carbon atoms include aryloxy groups having 6 to 20 carbon atoms such as a phenoxy group, a 2-methylphenoxy group, a 3-methylphenoxy group, a 4-methylphenoxy group, a 2,3dimethylphenoxy group, a 2,4-dimethylphenoxy group, a2,5-dimethylphenoxy group, a 2,6-dimethylphenoxy group, a 3,4-dimethylphenoxy group, a 3,5-dimethylphenoxy group, a 2,3,4-trimethylphenoxy group, a 2,3,5-trimethylphenoxy group, a 2,3,6-trimethylphenoxy group, a 2,4,5-trimethylphenoxy group, a 2,4,6-trimethylphenoxy group, a 3,4,5-trimethylphenoxy group, a 2,3,4,5-tetramethylphenoxy group, a 2,3,4,6-tetramethylphenoxy group, a 2,3,5,6-tetramethylphenoxy group, a pentamethylphenoxy group, an ethylphenoxy group, a n-propylphenoxy group, an isopropylphenoxy group, a n-butylphenoxy group, a sec-butylphenoxy group, a tert-butylphenoxy group, a n-hexylphenoxy group, a n-octylphenoxy group, a n-decylphenoxy group, a n-tetradecylphenoxy group, a naphthoxy group, and an anthracenoxy group. Specific examples

of the aryloxy group having 6 to 20 carbon atoms substituted with a halogen include the above aryloxy groups having 6 to 20 carbon atoms which are substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom or an iodine atom.
[0024] In substituents R1, R2, R3, R4, R5, and R6, specific examples of the aralkyloxy group having 7 to 20 carbon atoms include a benzyloxy group, a (2-methylphenyl)methoxy group, a (3-methyrphenyl)methoxy group, a (4-methylphenyl)methoxy group, a (2,3-dimethylphenyl)methoxy group, a (2,4-dimethylphenyl)methoxy group, a (2,5-dimethyrphenyl)methoxy group, a (2,6-dimethylphenyl)methoxy group, a (3,4-dimethylphenyl)methoxy group, a (3,5-dimethylphenyl)methoxy group, a (2,3,4-trimethyrphenyl)methoxy group, a (2,3,5-trimethylphenyl)methoxy group, a
(2,3,6_trimethylphenyl)methoxy group, a (2,4,5"trimethylphenyl)methoxy group, a (2,4,6-trimethylphenyDmethoxy group, a (3,4,5-trimethylphenyDmethoxy group, a (2,3,4,5-tetramethylphenyDmethoxy group, a (2,3,4,6-tetramethylphenyDmethoxy group, a
(2,3,5,6-tetramethylphenyOmethoxy group, a (pentamethylphenyl)methoxy group, an (ethylphenyl)methoxy group, a (n-propylphenyl)methoxy group, an (isopropylphenyl)methoxy group, a (n-butylphenyl)methoxy group, a (sec-butylphenyl)methoxy group, a (tert-butylphenyl)methoxy group, a (n-hexylphenyl)methoxy group, a (n-octylphenyl)methoxy group, a (n-decylphenyl)methoxy group, a naphthylmethoxy group, and an anthracenylmethoxy group, and preferably a benzyloxy group.
Specific examples of the aralkyloxy group having 7 to 20 carbon atoms substituted with a halogen include the abvove aralkyloxy groups which are substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom or an iodine atom.

[0025] In substituents R1, R2, R3, R4, R5, and Rs, the amino group substituted with a hydrocarbon group having 1 to 20 carbon atoms is an amino group substituted with two hydrocarbon groups, and examples of the hydrocarbon group include alkyl groups having 1 to 20 carbon atoms such as a methyl group, an ethyl group, a n-pxopyl group, an isopropyl group, a n-butyl group, a sec-butyl group, a tert-butyl group, an isobutyl group, a n-pentyl group, a n-hexyl group, and a cyclohexyl group, and aryl groups such as a phenyl group, and these substituents may be bonded together to form a ring. Examples of such an amino group substituted with a hydrocarbon group having 1 to 20 carbon atoms include a dimethylamino group, a diethylamino group, a di-n-propylamino group, a diisopropylamino group, a drn-butylamino group, a di-sec-butylamino group, a di-tertbutylamino group, a di-isobutylamino group, a tert-butylisopropylamino group, a di-nhexylamino group, a di-n-octylamirio group, a drndecylamino group, a diphenylamino group, a bistrimethylsilylamino group, abis-tert-butyldimethylsilylamirio group, a pyrrolyl group, pyrrolidinyl group, a piperidinyl group, a carbazolyl group, a dihydi'oindolyl group, and a dihydroisoindolyl group, and preferably a dimethylamino group, a diethylamino group, a pyrrolidinyl group, a piperidinyl group and the like.
Besides the above "described hydrocarbon groups, examples of the hydrocarbon group constituting these substituted amino groups include hydrocarbon groups substituted with a halogen atom such as a fluorine atom, a chlorine atom, a bromine atom, or an iodine atom.
[0026] R1 and R2 may be bonded together to form a ring, and adjacent two substituents among R3, R^, R5 and RG may optionally be bonded together to form a ring. [0027] Examples of the ring formed by bonding R1 andR2. and the ring

formed by bonding adjacent two substituents among R3, R4, R5 and RG
include saturated or unsaturated hydrocarbon rings substituted with a
hydrocarbon group having 1 to 20 carbon atoms. Specific examples thereof
include a cyclopropane ring, a cyclobutane ring, a cyclopentane ring, a
cyclohexane ring, a cycloheptane ring, a cyclooctane ring, a benzene ring, a
naphthalene ring, and an anthracene ring.
[0028] Examples of the rare earth metal complex (l) of the present invention
include the following complexes:
[l-(dimethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,3,4,5-
tetramethy ley clop entadienyl]bis (o N, N -dimethylaminob enzyl)scan dium,
[l-(diethyl{2-methoxy3-tert-butyl-5-methylphenyl}silyl)-2,3,4,5-
tetr amethylcycl op entadienyl]bis(o-N,N-dim ethylaminobenzyl) scan dium,
[l-(dimethyH2-methoxy-3-tert-butyl-5-methylphenyllsilyl)'
cyclop enta dienyl]bis(o -N, N - dimethylaminobenzyl) scan dium,
[l-(diethyl{2-methoxy3-tert-butyl-5-methylphenylfsilyl)-cyclopentadienyl]-
bis(o-N,N-dimethylaminobenzyl)scandium,
[l-(dimethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,4-dimethyl-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)scandium,
[l-(diethyl{2-methoxy-3-tert-butyl-5methylphenyl}silyl)-2,4-dimethyl-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)scandium,
[l-(dimethyH2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,3,5-trimethyl-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)scandium,
[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenyli'silyl)-2,3,5-trunethyl-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)scandium,
[0029]
[l-(dimethyH2-methoxy-3-tert-butyl-5-methylphenylSsilyl)-2.3.4,5-
tetr amethylcycl op entadi en yl]bis (trim ethylsilylmethyl) scan dium.
[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenylisilyl)-2.3.4.5-

tetr amethy ley clop entadienyljbis (trim ethylsilylmethyl) scandium,
[l-(dimethyH2-methoxy-3'tert-butyl-5-methylphenyl}silyl)cyclopentadienyl]-
bis (trimethylsilylm ethyl) scan dium,
[l-(diethyl{2-methoxy-3-tert-butyl'5-methylphenyl}silyl)cyclopentadienyl]-
bis(trimetbylsilylmethyl) scan dium,
[l-(dimethyl{2-methoxy-3'tert-butyl-5-methylphenyltsilyl)-2,4-dimethyl-
cyclop entadienyllbis (trimethylsilylmethyDscandium,
[l-(diethyl{2-methoxy3-tert-butyI-5-methylphenyIfsilyl}-2,4-dimethyI-
cyclopentadienyl]bis(trimethylsilylmethyl)scandium,
[l-(dimethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,3,5-trimethyl-
cyclop enta di en yl]bis(trim ethylsilylm ethyl)scan dium,
[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,3,5-trimethyl-
cyclopentadienyl]bis(trimethylsilylmethyi) scan dium,
[0030]
[l-(dimethyl{2-methoxy3-tertbutyl-5-methylphenyUsilyl)-2,3,4,5-
tetr amethylcyclop enta dienyl]bis (o -N, N - dimethylaminobenzyDlutetium,
[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,3,4,5-
tetrameth.ylcyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)lutetium,
[l-(dimethyl{2-methoxy3-tert-butyl-5-metbylphenyl}silyDcyclopentadienyl]-
bis(o-N,N-dimethylaminobenzyl)lutetium,
[l(diethyl{2-methoxy-3-tert-butyl-5-metbylphenyl}silyl)cyclopentadienyl]-
bis(o -N ,N - dimethylaminob enzyDlutetium,
[l-(dimethyl{2-methoxy3-tert-butyl-5-methylphenyl)-sily])-2,4-dimethyl-
cycl op entadienyl]bis(o-N.N-dimethylaminobenzyDlutetium,
[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2.4-dimethyl-
cyclopentadienyl]bis(o-N,N'dimethylaminobenzyl)lutetium,
El-(dimethyl{2-methoxy-3-tert-butyl'5-methylphenyl}silyl)-2,3.5-trimethyl-
cydopentadienyl]bis(o-N.N-dimethylaminobenzy])lutetium.

[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2)3,5-trimethyl-
cyclopentadienyl]bis(o~N,N-dimethylaminobenzyl)lutetium,
[0031]
[l-(dimethyl{2-metlioxy-3-tert-butyl-5-methylphenyl}silyl)-2,3,4,5-
tetramethylcyclopentadienyl]bis(trimetliylsilylmetbyl)lutetium,
[l-(diethyl{2-methoxy-3-tert-butyl-5-metliylpbenyl}sLlyl)-2,3,4,5-
tetr amethylcyclop enta dienyllbis (trimethylsilylmethyl)lutetium,
[l-(dimethyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)cyclopentadienyl]-
bis(trimethylsilylmethyl)lutetium,
[l-(dietbyl{2-methoxy3-tert-butyl-5-methylphenyl}silyl)cyclopentadienyl]'
bis (trim ethylsilylmethyDlutetium,
[l'(dimetbyl{2-methoxy-3-tert-butyl-5-methylphenyl}silyl)-2,4-dimethyl-
cyclop enta dienyl]bis(trimethylsilylmethyl)lutetium,
[l-(diethyl{2-methoxy-3-tert-butyl-5-methylphenyllsilyl)-2,4-dimetbyl'
cyclop entadienyl]bis (trimethylsilylmethyl)lutetium,
[l-(dimethyl{2-methoxy-3-tert-butyl-5-methyIphenylisilyI)-2,3,5-trimethyI-
cyclop entadienyl]bis(trimethylsilylmetliyl)lutetium,
[l-(diethyl!2-methoxy3-tert-butyl-5-methyIphenyI}silyl}-2,3,5-trimetbyI-
cyclopentadienyl]bis(trimethylsilylmethyl)lutetium,
[0032]
[ 1- {1 • (2 -methoxy- 3 -tert-butyl- 5 -methylphenyl) - 1-methylethyl}-
cyclop entadienyl]bis(o -N,N - dimethylaminobenzyDy ttrium,
[l-{l-(2-methoxy3-tert-butyl-5-metliylphenyl)-l-ethylpropyl}-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyI)yttrium,
[l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethylK3-methyl'
cyclop en ta di en yl]bis(o-N,N- dimethylaminobenzyDy ttrium,
[l'U-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-ethylpropyU-3-methyl-
cyclopentadienyl]bisfo-N,N-dimethylaniinobenzyl)yttrium.

[l-{l-{2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethylf-3-tert'butyl-
cyclopentadienyl]bis(o_N,N-dimethylaminobenzyl)yttrium,
[l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-ethylpropyl}-3-tert-butyl-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)yttrium,
[0033]
[l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyl}-
cyclop entadienyllbis (trim ethylsUylmethyl)yttrium,
[l-{l-(2-methoxy3-tert-butyl-5-methylphenyl)-l-ethylpropyl}-
cyclop entadienyllbis (trimethylsilylm ethyl) yttrium,
[l'{l-(2-methoxy3-tert-butyl-5-methylphenyl)-l-methylethylf-3-methyl-
cyclop entadienyl]bis(trimethylsilylmethyl)y ttrium,
[l-{l-(2'methoxy-3-tert'butyl-5-methylphenyl)-l-ethylpropyl}-3-methyl-
cyclop entadi en yl]bis(trimethylsilylm ethyl) yttrium,
[l-{l-(2-methoxy3-tert-butyl-5-methylphenyl)-l-methylethy}-3-tert-butyl-
cyclop entadienyl3bis(trimethylsilylmethyl)yttrium,
[l-tl-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-ethypropyli--3-tert-butyl-
cyclop enta dienyllbis (trimethylsilylmethyOyttrium;
as well as the above compounds in which scandium, lutetium or yttrium is
replaced by lanthanum, cerium, praseodymium, neodymium, promethium,
samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium,
thulium or ytterbium.
[0034] The rare earth metal complex (l) can be produced by reacting the
cyclopentadiene compound (2) and the rare earth metal compound
represented by the formula (3) (hereinafter, abbreviated as a rare earth
metal compound (3)).
[0035] Examples of the hydrocarbon group having-1 to 20 carbon atoms in
the alkyl group optionally substituted with a silyl group substituted with a
hydrocarbon group having 1 to 20 carbon atoms in the substituent R8 include

a methyl group, an ethyl group, a n-propyl group, an isopropyl group, a n-butyl group, a sec-butyl group, a tert-butyl group, a n-pentyl group, a neopentyl group, an amyl group, a n-hexyl group, a heptyl group, a n-octyl group, a n-nonyl group, a n-decyl group, a n-dodecyl group, a n-tridecyl group, a tetradecyl group, a pentadecyl group, a hexadecyl group, a heptadecyl group, an octadecyl group, a nonadecyl group, and a n-eicosyl group, and preferably a methyl group, an ethyl group, an isopropyl group, a tert-butyl group, an amyl group and the like.
[0036] Examples of the aikyl group optionally substituted with a silyl group substituted with a hydrocarbon group having 1 to 20 carbon atoms in the substituent R8 include a trimethylsilylmethyl group, a triethylsilylmethyl group, a triisopropylsilylmethyl group, a trrnbutylsilyrmethyl group, and a tert-butyldimethylsilylmethyl group, and preferably a trimethylsilylmethyl group.
[0037] Examples of the hydrocarbon group having 1 to 20 carbon atoms in the araLkyl group substituted with an amino group substituted with a hydrocarbon group having 1 to 20 carbon atoms in the substituent R8 include a methyl group, an ethyl group, a n-propyl group, an isopropyl group, a n-butyl group, a sec-butyl group, a tert-butyl group, a n-pentyl group, a neopentyl group, an amyl group, a n-hexyl group, a heptyl group, a n-octyl group, a n-nonyl group, a n-decyl group, a n-dodecyl group, a n-tridecyl group, a tetradeyl group, a pentadecyl group, a hexadecyl group, a heptadecyl group, an octadecyl group, a nonadecyl group, and a n-eicosyl group, and preferably a methyl group, an ethyl group, an isopropyl group, a tert-butyl group, an amyl group and the like.
[0038] Examples of the aralkyl group substituted with an amino group substituted with a hydrocarbon group having 1 to 20 carbon atoms in the substituent Ra include an o-N.N-dimethylaminobenzyl group, and an

o-N,N-diethylamiiiobenzyl group, and preferably an o-N,N-dimethylamino-benzyl group.
[0039] The cyclop entadiene compound (2) may be produced by, for example, a known method (see JP-A-09-87313).
[0040] Examples of such a cyclop entadiene compound (2) include the following compounds^
(2-methoxyphenyl)(cyclopentadienyl)diethylsilane, (2-methoxy-3-methylphenyl)(cyclopentadienyl)diethylsilane, (2-methoxy3,5-dimethylphenyl)(cyclopentadienyl)diethylsilane, (2-methoxy-3-tert-butylphenylXcyclopentadienyl) diethylsilane, (2-methoxy3-tert-butyl-5Tnethylphenyl)(cyclopentadienyl)diethylsilane, (2 -methoxy -3,5 - di-tert-butylphenyl) (cyclop entadienyl) diethylsilane, (2-methoxy-5-methyl-3-phenylphenyl)(cyclopentadienyl)diethylsilane, (2-methoxy-5-methyl-3-trim ethylsilylphenyl)(cyclop entadienyl) diethylsilane, (2-methoxy-3-tert-butyldimethylsilyl-5-methylphenyl)(cyclopentadienyl)' diethylsilane,
(2-methoxy-3,5-diamylphenyl)(cyclopentadienyl)diethylsilane, (2-methoxy-3-tert-butyl-5-methoxyphenyl)(cyclopentadienyl)diethylsilane, (2-methoxy-5-tert-butyl-3-chlorophenyl)(cyclopentadienyl) diethylsilane, (l-methoxynaphthalen-2-yl)(cyclopentadienyl) diethylsilane, (2-methoxy-3-tert-butyl-5-methoxyphenyl)(cyclopentadienyl)dietliylsiIane, [0041]
(2-methoxyphenyl(2,3,4,5-tetramethylcyclopentadienyl) diethylsilane, (2-methoxy3-methylphenyl) (2,3,4,5-te tr am ethylcyclop entadienyl) diethyl¬silane,
(2-methoxy 3,5-dimethylphenyl)(2,3,4,5-tetramethylcyclopentadienyl)" diethylsilane, (2-methoxy3-tert-butylphenyl)(2,3,4.5-tetramethylcyclopentadienyl)diethyl-

silane, (2-methoxy-3-tert-butyl-5-methylphenyl)(2,3,4,5-tetramethyl-
cyclop enta dienyl) diethylsilane,
(2-methoxy-3,5-di-tert-butylphenyl)(2,3,4,5-tetramethylcyclopentadienyl)-
diethylsilane,
(2-methoxy-5-methyl-3-phenylphenyl)(2,3,4,5-tetramethylcyclopentadienyl)-
diethylsilane,
(2-methoxy5'methyl-3-trimethylsilylphenyl)(2,3,4,5-tetramethyl-
cyclopentadienyOdiethylsilane,
(2-methoxy3-tert-butyldimethylmethylsilyl-5-methylphenyl)(2,3,4,5"
tetramethylcyclopentadienyDdiethylsilane,
(2-meth.oxy-3,5-diamylpbenyl)(2,3,4,5-tetramethylcyclopentadienyl)diethyl-
silane, (2-methoxy-3-tert-butyl-5-methoxyphenyl)(2,3>4,5-tetramethyl-
cyclopentadienyDdiethylsilane,
(2-metboxy5'tert-butyl-3-chlorophenyD(2,3,4,5_tetrametbyl-
cyclopentadienyDdiethylsilane,
(l-methoxynaphthalen-2-yl)(2,3,4,5-tetrametbylcyclopentadienyDdiethyl-
silane, (2-methoxy3-tert-butyl-5-methoxyphenyl)(2,3,4,5-tetramethyl-
cyclopentadienyl)diethylsilane, and the like;
as well as the above in which diethylsilane is replaced by dimethylsilane,
diphenylsilane, ethylmethylsilane, methylphenylsilane, dimethylmethane,
or diethylmethane,
[0042]
2 - [ 1 - (cyclop entadienyl)-1 -methylethyl] - 1-methoxybenzene,
2-[l-(cydopentadienyl)-l-methylethyl]-l-methoxy-4,6_dimethylbenzene,
6-tert-butyl-2-[l-(cy clopentadienyl)-l-methylethyl]-1-methoxy-4-methyl-
benzene, 6-[l-(cyclopentadienyl)-l-methylethyl]-l-methoxy2-phenylbenzene,
l-tert-butyldimethylsilyl-3-[l-(cyclopentadienyl)-l-methylethyl]-2-methoxy-
5-methylbenzene,

3-[l *(cyclopentadienyl)-l-methylethyl]-2-methoxy-5-methyl-1-trimethylsilyl-
benzene,
6-tert-butyl-2-[l-(cyclopentadienyl)-l-methylethyl]-1,4-dimethoxybenzene,
5-tert-butyM-chloro-3-[l-(cyclopentadienyl)-l-methylethyl]-4-methoxy-
benzene,
6-tert-butyl-2-[l-(cyclopentadienyl)-l-methylethyl]-l-methoxybenzene,
l-methoxy-2-[l-(4-methyl-cyclopentadienyl)-l-methylethyl]benzene,
l-methoxy-4,6-dimethyl-2^[l-(4-methyl-cyclopentadienyl)l-methylethyl]-
benzene,
6-tert'butyl-l-methoxy-4-methyl-2-[l-(4-methyl-cyclopentadienyl)-l-methyl-
ethyllbenzene,
l-methoxy-6-[l-(4-methyl-cyclopentadienyl)-l-methylethyl]-2-phenylbenzene,
l-tert-butyldimethylsilyl-2-methoxy-5-methyl-3-El-(4-methyl-
cyclopentadienyl)-l-methylethyl]benzene,
2-methoxy5-methyl-3-[l-(4-methyl-cyclopentadienyl)-lmethylethyl]-l-
trimethylsilylbenzene,
6-tert-butyll,4-dimethoxy-2-[l-(4-methyl-cyclopentadienyl)l-methylethyl]-
benzene,
5-tert-butyM-chloro-4-methoxy-3-[l-(4-methyl-cyclopentadienyl)-l-methyl-
ethyl]benzene,
6-tert-butyl-l-methoxy-2-[l-(4-methyl-cyclopentadienyl)-l-methylethyl]-
benzene,
2 - [ 1 (4-tert-butyl-cyclopentadienyl)-1 -methylethyl] -1 -methoxybenzene,
2-[l(4'tert-butyl-cyclopentadienyl)-l-methylethyl]-l-methoxy-4,6-dimethyl-
benzene,
6-tert-butyl-2-[l-(4-tert-butyl-cyclopentadienyl)-1 -methylethyl]- 1-methoxy
4 -methylbenzene,
6-[l-(4-tert.-butyl-cyclopentadienyl)-l-methylethyl]-l-methoxy-2-phenyl-

benzene,
l-tert-butyldimethylsilyl-3-[l-(4-tert-butyl-cyclopentadienyl)-l-methylethyl]-
2-methoxy5'methylbenzene,
3-[l-(4-tert-butylcyclopentadienyl)-l-methylethyl]-2-methoxy-5-methyl-l-
trimethylsilylbenzene,
6-tert-butyl-2-[l-(4-tert-butyl-cyclopentadienyl)-l-methylethyl]-l,4-
dimethoxyb enzene,
5-tert-butyl-l-chloro-3-[l-(4-tert-butyl-cyclopentadienyl)-l-methylethyl]-4-
methoxybenzene,
6-tert-butyl-2-[l-(4-tert-butyl-cyclopentadienyl)-l-methylethyl]-lmethoxy-
benzene and the like;
as well as the above compounds in which methoxy is replaced by ethoxy,
isopropoxy, phenoxy, or benzyloxy.
[0043] Examples of the monoanionic ligand represented by the substituent
X in the rare earth metal complex (l) and the rare earth metal compound (3)
include a hydrogen atom, a halogen atom, a methyl group, an ethyl group, a
n-butyl group, a neopentyl group, a phenyl group, a neopentylidene group, a
methoxy group, a tert-butoxy group, a phenoxy group, a benzyl group, an
amide group, a phosphino group, a trimethylsilylmethyl group, a
bis(trimethylsilyl)methyl group, a bis(trimethylsilyl)amide group, and an
o-dimethylaminobenzyl group, and preferably a methyl group, a
trimethylsilylmethyl group, and an o-dimethylaminobenzyl group.
[0044] When m is 2, two Xs may be bonded together, or may be taken
together to form a dianionic ligand.
[0045] Examples of the neutral ligand represented by the substituent Y in
the rare earth metal complex (l) and the rare earth metal compound (3)
include olefins, aromatic compounds, ethers, sulfides, amines, nitriles.
phosphines. andphosphine oxides, and preferably ethers and amines.

Specific examples of the neutral ligand represented by Y include ethylene, propylene, 1-butene, cyclooctadiene, styrene, benzene, toluene, naphthalene, anthracene, diethyl ether, tetrahydrofuran, 1,2-dimethoxyethane, dimethyl sulfide, thiophene, tetrahydrothiophene, trimethylamine, triethylamine, ethyldiisopropylamine, N,N- dim ethyl aniline, N,N,N',N'-tetramethylethylenediamine, pyridine, N,N-dimethylaminopyridine, acetonitrile, trimethylphosphine, triethylphosphine, tri-tert-butylphosphine, tricyclohexylphosphine, triphenylphosphine, trimethylphosphine oxide, and triphenylphosphine oxide, and preferably tetrahydrofuran, diethyl ether, N,N'dimethylanihne, and trimethylphosphine. [0046] X and Y may be bonded together to form a multidentate ligand.
Specific examples of the multidentate ligand include an o-N,N-dimethylaminoben£yl group.
[0047] In the formulae (l) and (3), m represents an integer of 1 to 3, preferably 1 or 2, more preferably 2, and n represents an integer of 0 to 3, preferably 0 to 2, more preferably 0 or 2.
[0048] Such a rare earth metal compound (3) may be synthesized by a known process (see J. Am. Chem. Soc, 1978, 100, 8068, or J. Chem. Soc, Chem. Comm., 1973, 126).
[0049] Examples of such a rare earth metal compound (3) include tris(trimethylsilylmethyl) scan drum,
tris(o-N,N-dimethylaminobenzyl)scandium and the like, and may be adducts of these compounds with diethyl ether, tetrahydrofuran, trimethylamine, triethylamine, N.N-dimethyl aniline and N.N,N\N'-tetramethylethylene-diamine. Additional examples include the above compounds in which scandium is replaced by yttrium, lanthanum, cerium, praseod3rmium, neodymium. promethium. samarium, europium, gadolinium, terbium.

dysprosium, holmium, erbium, thulium, ytterbium or lutetium. More preferable examples include tris(o-N,N-dimethylaminobenzyl)scandium, tris(o-N,N-dimethylaminobenzyl)yttrium, and tris(o-N,N-dimethylaminobenzyl)lutetium.
[0050] A reaction between the cyclopentadiene compound (2) and the rare earth metal compound (3) may be usually performed by adding the cyclop entadiene compound (2) to a solvent followed by the addition of the rare earth metal compound (3).
[0051] An amount of the rare earth metal compound (3) is usually 0.5 to 3 moles, preferably 0.7 to 1.5 moles per 1 mole of the cyclop entadiene compound (2).
[0052] A reaction temperature is usually from - 100°C to the boiling point of a solvent, preferably in a range of -80°C to 60°C.
[0053] The reaction is usually performed in a solvent inert to the reaction. Examples of such a solvent include aromatic hydrocarbons such as benzene and toluene; aliphatic hydrocarbons such as hexane and heptane; ethers such as diethyl ether, tetrahydrofuran, and 1,4-dioxane; amides such as hexamethylphosphoric amide, and dimethyIformamide; polar solvents such as acetonitrile, propionitrile, acetone, diethyl ketone, methyl isobutyl ketone, and cyclohexanone; and aprotic solvents such as halogenated solvents such as dichloromethane, dichloroethane, chlorobenzene and dichlorobenz^ne. Such solvents may be used alone or as a mixture of two or more of them, and an amount thereof is usually 1 to 200 parts by weight, preferably 3 to 50 parts by weight per 1 part by weight of the cyclop entadiene compound (2). [0054] After the completion of the reaction, an desired rare earth metal complex (l) can be obtained from the resultant reaction mixture by a conventional method, for example, by filtering the produced precipitate, concentrating the filtrate to precipitate a rare earth metal complex (l). and

collecting the complex by filtration. [0055] [Catalyst for olefin polymerization]
The catalyst for olefin polymerization of the present invention is a catalyst for olefin polymerization comprising the rare earth metal complex (l) as a component of the catalyst for olefin polymerization, and is obtained by contacting the rare earth metal complex (l) with other co-catalytie component. Examples of the catalyst for olefin polymerization include catalysts for olefin polymerization obtained by contacting the rare earth metal complex (l) with at least one compound selected from the group consisting of the following aluminum compounds (Al) to (A3) and the following boron compounds (BlJ to (B3); Aluminum .compounds (A): (Al): an organoaluminum compound represented by the formula:
(E0aAlz (3-ai;
(A2): a cyclic aluminoxane having a structure represented by the formula:
{-Al(E2)-0-}b; and (A3): alinear aluminoxane having a structure represented by the formula:
E3{-Al(E3)-0-KAl(E3)2 wherein a represents a number satisfying 0 BQ'Q2Q3; (B2): a boron compound represented by the formula:

G+(BQiQ2Q3Q4)-; and (B3): a boron compound represented by the formula:
(L'-H)+(BQ>Q2Q3Q4)" wherein B represents a boron atom in the trivalent state, Q1, Q2, Q3 and Q4 each represent independently a halogen atom, a hydrocarbon group, a halogenated hydrocarbon group, a substituted silyl group, an alkoxy group or a di-substituted amino group, G+ represents an inorganic or organic cation, and L1 represents a neutral Lewis base.
[0056] Examples of the organoaluminum compound (Al) represented by the formula^ (EOaAlZa-a) include trialkylaluminums such as trimethylaluminum, triethylaluminum, tripropylaluminum, triisobutylalurninum, and trihexylaluminum; dialkylaluminum chlorides such as dimethylaluminum chloride, diethylaluminum chloride, dipropylaluminum chloride, diisobutylaluminum chloride, and dihexylaluminum chloride; alkylaluminum dichlorides such as methyl aluminum dichloride, etiiylaluminum dichloride, propylaluminum dichloride, isobutylaluminum dichloride, and hexylaluminum dichloride.' dialkylaluminum hydrides such as dimethylaluminum hydride, diethylaluminum hydride, dipropylaluminum hydride, diisobutylaluminum hydride, and dihexylaluminum hydride. Preferable is trialkylaluminum, and more preferable is triethylaluminum or triisobutylalurninum. [0057] Examples of E2 and E3 in the cyclic aluminoxane (A2) having a structure represented by the formula: {-Al(E2)-0-h, or the linear aluminoxane (A3) having a structure represented by the formula: E3{-Al(E3)-0-}cAl(E3)2 include alkyl groups such as a methyl group, an ethyl group, a n-propyl group, an isopropyl group, a n-butyl group, an isobutyl group, a n-pentyl group, and a neopentyl group. Here, b is an integer of at least 2, and c is an integer of at least 1. Preferably, E2 and E3 are each independently a methyl

group or an isobutyl group, b is 2 to 40, and c is 1 to 40. [0058] The aluminoxane is prepared by a variety of processes. The process is not particularly limited, and the aluminoxane may be prepared by a known method. For example, the aluminoxane is prepared by contacting a solution of a trialkylaluminum (e.g. trimethylaluminum) dissolved in an appropriate organic solvent (benzene or an aliphatic hydrocarbon) with water. Additional examples include a method of contacting a trialkylaluminum (e.g. trimethylaluminum) with a metal salt containing crystal water (e.g. copper sulfate hydrate).
[0059] In the boron compound (Bl) represented by the formula: BQ*Q2Q3, B is a boron atom in the trivalent state. Q1 to Q3 each are independently, preferably, a halogen atom, a hydrocarbon group having 1 to 20 carbon atoms, a halogenated hydrocarbon group having 1 to 20 carbon atoms, a substituted silyl group having 1 to 20 carbon atoms, an alkoxy group having 1 to 20 carbon atoms or a disubstituted amino group having 2 to 20 carbon atoms, more preferably a halogen atom, a hydrocarbon group having 1 to 20 carbon atoms, or a halogenated hydrocarbon group having 1 to 20 carbon atoms. [0060] Examples of the boron compound (Bl) represented by the formula: BQLQ2Q3 include tris(pentafluorophenyl)borane,
tris(2,3,5,6-tetrafluorophenyl)borane, tris(2,3,4,5-tetrafluorophenyI)borane, tris(3,4,5trifLuorophenyl)borane, tris(2,3,4-trifTuorophenyl)borane, phenylbis(pentafluorophenyl)borane and the like, and preferably tris(pentafluorophenyl)borane.
[0061] In the boron compound (B2) represented by the formula' G+(BQ'Q2Q3Q4)~, G+ is an inorganic or organic cation, B is a boron atom in the trivalent state, and Q' to Q-* are the same as defined for Q1 to Q3 in the (Bl). [0062] In the boron compound (B2) represented by G+(BQ^Q^)",

examples of inorganic cation G+ include a ferrocenium cation, an
alkyl-substituted ferrocenium cation, and a silver cation, and examples of
organic cation G+ include a triphenylmethyl cation. Examples of
(BQ1Q3Q3Q4)" include tetrakis(penta£luorophenyl)borate,
tetrakis(2,3,5,6-tetrafluorophenyl)borate,
tetrakis(2,3,4,5"tetrafluorophenyl)borate,
tetrakis(3,4,5-trifluorophenyl)borate, tetrakis(2,2,4-trifluoroprienyl)borate,
phenylbis(pentafLuorophenyl)borate, and
tetrakis(3,5-bistrifluoromethylphenyl)borate.
[0063] Examples of the boron compound (B2) represented by the formula:
G+(BQ'Q2Q3Q4)" include ferrocenium tetrakis(pentafluorophenyl)borate,
l,l'-dimethylferrocenium tetrakis(penta£Luorophenyl)borate, silver
tetrakis(pentafluorophenyl)borate, triphenybnethyl
tetrakis(pentafl.uorophenyl)borate, and triphenylmethyl
tetrakis(3,5-bistrifluoromethylphenyl)borate, and preferably
triphenylmethyl tetrakis(pentafluorophenyl)borate.
[0064] In the boron compound (B3) represented by the formula:
(L,-H)+(BQ1Q5Q3Q-i)-, LI ^ a neutral Lewis base, G>H)+ is a Brensted acid,
B is a boron atom in the trivalent state, and Q1 to Q4 are the same as as
defined for Q1 to Q3 in the [0065] In the boron compound (B3) represented by the formula:
(Li-HHBQJQ^Q-O ", examples of 0>H)+ include trialkyl-substituted
ammonium, N,N'diaUtylaniHnium, dialkylammonium, and
triarylphosphonium, and examples of (BQ'Q2Q3Q4)~ include the same
cations as those described above.
[0066] Examples of the boron compound (B3) represented by the formula:
(L1-H)+(BQiQ^Q3Q4)- inciude triethylammonium
tetraids(pentafluorophenylborate, tripropylammonium

tetrakis(pentafluorophenyl)borate, tri(normalbutyl) ammonium
tetrakis(pentafluorophenyl)borate, tri(normalbutyl) ammonium
tetralds(3,5-bistrifluoromethylphenyl)borate, N,N-dimethylanilinium
tetrakis(pentafluorophenyl)borate, N,N-diethylanilinium
tetr aids (pentaflu or ophenyl)borate. N,N-2,4,6_pentamethylanilinium
tetralds(pentafruorophenyl)borate, N.N-dimethylanilinium
tetrakis(3,5"bistrifluoromethylphenyl)borate, diisopropylammonium
tetraids(pentafluorophenyl)borate, dicyclohexylammonium
tetrakis(pentafluorophenyl)borate, triphenylphosphonium
tetr aids (pentafruorophenyl)bor ate, tri(methylphenyl)phosphonium
tetrakis(pentafluorophenyl)borate, and tri(dimethylphenyl)phosphonium
tetrakis(pentafluorophenyl)borate, and preferably
tri(normalbutyl)ammonium tetrakis(pentafluorophenyl)borate and
N,N-dimethylanilinium tetrakis(pentafluorophenyl)borate.
[0067] As the compound (B), usually any one of the boron compound (Bl)
represented by the formula- BQ^Q3, the boron compound (B2) represented
by the formula^ G+(BQ!Q2Q3Q4) ~ and the boron compound (B3) represented
by the formula: (L,-H)+(BQiQ2Q3Q-')" is used.
[0068] In the method of contacting catalytic components with each other in
production of the catalyst for olefin polymerization, any two catalytic
components may be contacted with each other in advance and, thereafter, the
remaining catalytic component may be contacted therewith- Alternatively,
catalytic components may be contacted with each other in a polymerization
reactor, or respective catalytic components may be separately charged into a
polymerization reactor in an arbitrary order, or arbitrary two or more
catalytic components which have been contacted with each other in advance
may be charged therein.
[0069] Regarding the amount of the catalytic components, the molar ratio of

the compound (A) (in terms of aluminum atom) to the rare earth metal complex (l) is usually 0.1 : 1 to 10000 : 1, preferably 5 : 1 to 2000 : 1. When the organoaluminum compound (Al) is used as the compound (A), the molar ratio of the compound (A) to the rare earth metal complex (l) is more preferably 0.3 : 1 to 500 '■ 1, further preferably 0.5 ' 1 to 100 '■ 1. In addition, the molar ratio of compound (B) to the rare earth metal complex (l) is usually 0.01 : 1 to 100 : 1, preferably 0.5 : 1 to 10 : 1.
[0070] Regarding a concentration when each catalytic component is used in a solution state, the concentration of the rare earth metal complex (l) is usually 0.0001 to 5 mmol/liter, preferably 0.001 to 1 mmol/liter, the concentration of the compound (A) in terms of an aluminum atom is usually 0.01 to 500 mmol/liter, preferably 0.1 to 100 mmol/liter, and the concentration of the compound (B) is usually 0.001 to 5 mmol/liter, preferably 0.001 to 1 mmol/liter. [0071] [Process for producing olefin polymer]
In the process for producing the olefin polymer of the present invention, an olefin is polymerized in the presence of the catalyst for olefin polymerization comprising the rare earth metal complex (l) as a component of the catalyst for olefin polymerization.
[0072] As the olefin used in polymerization, a linear olefin, a cyclic olefin and the like may be used, and a single olefin is homopolymerized, or two or more olefins are copolymerized. Usually, an olefin having 2 to 20 carbon atoms is used.
[0073] Examples of the linear olefin include ethylene! a-olefrns having 3 to 20 carbon atoms such as propylene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 1-nonene, 1-decene, 3-methyM-pentene, 4-methyM-pentene, 3.3■dimethyl-1-butene, 5-methyl- 1-hexene, and 3,3-dimethyl-1-pentene: non-conjugated dienes such as 1,5-hexadiene.

1,4-uexadiene, 1,4-pentadiene, 1,5-heptadiene, 1,6-heptadiene, 1,6-octadiene, 1,7-octadiene, 1,7-nonadiene, 1,8-nonadiene, 1,8-decadiene, 1,9-decadiene, 1,12-tetradecadiene, 1,13-tetradecadiene, 4-methyl-l,4-hexadiene. 5-methyl-l,4-hexadiene, 7-methyl-1,6-octadiene, 3-methyl-l,4-hexadiene, 3-methyl-l,5-hexadiene, 3-ethyl-l,4-hexadiene, 3-ethyM,5-hexadiene, 3,3-dimethyll,4-hexadiene, and 3,3-dimethyl-l,5-hexadiene; conjugated dienes such as 1,3-butadiene, isoprene, 1,3-hexadiene, and 1,3-octadiene. [0074] Examples of the cyclic olefin as an alicyclic compound include monoolefins such as vinylcyclopentane, vinylcyclohexane, vinylcycloheptane, norbornene, 5-methyl'2-norbornene, 5-ethyl-2-norbornene, 5-butyl"2-norbornene, tetracyclododecene, tricyclodecene, tricycloundecene, pentacyclopentadecene, pentacyclohexadecene, 8-methyltetracycIododecene, and 8-ethyltetracyclododecene; non-conjugated dienes such as 5-ethylidene-2-norbornene, dicyclopentadiene, 5-vinyl-2-norbornene, norbornadiene, 5-methylene-2-norbornene, 1,5-cyclooctadiene, 7-methyl-2,5-norbornadiene, 7-ethyl-2,5-norbornadiene, 7-propyl-2,5-norbornadiene, 7-butyl-2,5-norbornadiene, 7-pentyl-2,5-norbornadiene, 7-hexyl-2,5-norbornadiene, 7,7-dimethyl-2,5-norbornadiene, 7,7-methylethyl-2,5-norbornadiene, 7chloro-2,5-norbornadiene, 7-bromo-2,5-norbornadiene, 7-fLuoro-2,5norbornadiene, 7T7-dichloro-2,5-norbornadiene, l-methyl-2,5-norbornadiene, l-ethyl-2,5-norbornadiene, l-propyl-2,5-norbornadiene, l-butyl-2,5-norbornadiene, l-chloro-2,5-norbornadiene, l-bromo-2,5norbornadiene, 5.8-endomethylenehexahydronaphthalene, and vinylcyclohexene; conjugated dienes such as 1,3-cyclooctadiene, and 1,3-cyclohexadiene. In addition, examples of the aromatic compound include styrene, o-methylstyrene, m-methylstyrene. p-methylstyrene, o,p-dimethylstyrene, o-ethylstyrene,

m-ethylstyrene, p-ethylstyrene, a-methylstyrene, and divinylbenzene. [0075] Examples of the combination of olefins when olefins are copolymerized include combinations of linear olefin/Iinear olefin such as ethylene/propylene, ethylene/1-butene, ethylene/1-hexene, ethylene/propylene/1-butene, ethylene/propylene/ 1-hexene, propylene/1-butene, and propylene/1-hexene 1 combinations of linear olefm/cyclic olefin such as ethylene/vinylcyclohexane, ethylene/norbornene, ethylene/tetrachlorododecene, ethylene/5-ethylidene-2-norbornene, propylene/vinylcyclohexane, propylene/norbornene,
propylene/tetracyclododecene, propylene/5-ethylidene-2-norbornene, and ethylene/propylene/5-ethylidene-2-norbornene.
[0076] The polymerization process is not particularly limited, and for example, solution polymerization or slurry polymerization using an aliphatic hydrocarbon (butane, pentane, hexane, heptane, octane or the like), an aromatic hydrocarbon (benzene, toluene or the like) or a halogenated hydrocarbon (methylene dichloride or the like) as a solvent, vapor phase polymerization in a gaseous monomer or the like is possible, and either continuous polymerization, or batch polymerization is possible. [0077] A polymerization temperature is usually in a range of-50°C to 300°C, particularly in a range of-20°C to 250°C. Apolymerization pressure is preferably an atmospheric pressure to 90 MPa. In general, a polymerization time is determined appropriately depending on the kind of the intended polymer, and a reactor, and a time in a range of 1 minute to 20 hours may be adopted. Furthermore, in the present invention, a chain transfer agent such as hydrogen may be added in order to adjust the molecular weight of a polymer. [0078]
Using the rare earth complex (l) of the present invention, a polar

monomer may be homopolymerized, or a certain polar monomer and a different polar monomer may be copolymerized. The kind of the polar monomer is not particularly limited, and examples thereof include lactones, alkylene oxides, (meth)acrylate esters and the like. [0079] [Process for producing lactone polymer]
Examples of the lactones used in the present invention include p-propiolactone, ybutyrolactone, 5-valerolactone, e-caprolactone, p-methylpropiolactone, 3,3.5-trimethyl-e-caprolactone and the like, and preferably e-caprolactone.
[0080] These lactones may be polymerized alone while a mixture of two or more lactones may be copolymerized. A method of copolymerizing two or more lactones is not particularly limited, and examples thereof include a method of initiating polymerization under such a condition that two or more lactones are present simultaneously to obtain a random copolymer, and a method of polymerizing the first lactone in advance, and then adding the second or subsequent lactone(s) to obtain a block copolymer. [0081] The polymerization method is not particularly limited, and for example, solution polymerization or slurry polymerization using an aliphatic hydrocarbon (butane, pentane, hexane, heptane, octane or the like), an aromatic hydrocarbon (benzene, toluene or the like) or a halogenated hydrocarbon (methylene dichloride or the like) as a solvent can be employed, and either continuous polymerization or batch polymerization is possible. [0082] Apolymerization temperature is usually in a range of -80°C to 150°C, particularly in a range of -30°C to 100°C. In general, a polymerization time is determined appropriately depending on the kind of the intended polymer. and a reactor and, for example, a time in a range of 1 second to 24 hours can be adopted. [0083] Preferably, the polymerization reaction is performed under an

atmosphere of an inert gas such as nitrogen or argon. It is important for
the efficient preparation of a polymer that the inert gas and the lactone
monomer are sufficiently dried so as to be free from water.
[0084] The resultant lactone polymer contains a metal catalytic component.
However, when a polymerization degree is high, it is not necessary to remove
the metal catalytic component since the content of the contained metal
catalytic component is relatively small. When the removal of the metal
catalytic component is necessary, the lactone polymer as produced is washed
with water or dilute hydrochloric acid to remove the metal catalytic
component, followed by drying, to obtain the lactone polymer containing no
metal catalytic component.
[0085] It is possible to produce a polymer of lactones of the present invention
at a relatively low temperature. In this case, the polymer has such
characteristics that it has excellent color tone, and little odor, since the
amount of mixed impurities generated by depolymerization or thermal
degradation of the lactone polymer is small.
[0086] The resultant lactone polymer may be pelletized with an extruder,
and can be used as a film, a fiber, an expanded sheet or various molded
articles.
[0087] [Process for producing alkylene oxide polymer]
Examples of the alkylene oxide used in the present invention include crolefin oxides having 2 to 9 carbon atoms such as ethylene oxide, propylene oxide, butyiene oxide, cyclohexene oxide, cycloheptene oxide, and cyclooctene oxide, a-olefm oxides having 10 or more carbon atoms, styrene oxide, and epichlorohydrin.
[0088] These alkylene oxides may be polymerized alone, while a mixture of two or more alkylene oxides may be copolymerized. A method of

copolymerizing two or more alkylene oxides is not particularly limited, and examples thereof include a method of initiating polymerization under such a condition that two or more alkylene oxides are present simultaneously to obtain a random copolymer, and a method of polymerizing the first alkylene oxide in advance, and then adding the second or subsequent alkylene oxide(s) to obtain a block copolymer.
[0089] A method of initiating polymerization is not particularly limited. For example, an alkylene oxide is added to the solution of the rare earth metal complex (l) to initiate polymerization, or the rare earth metal complex (l) is added to the solution of an alkylene oxide to initiate polymerization. [0090] A polymerization method is not particularly limited, and solution polymerization or slurry polymerization using an aliphatic hydrocarbon (butane, heptane, hexane, heptane, octane or the like), an aromatic hydrocarbon (benzene, toluene or the like), an ether (diethyl ether, tetrahydrofuran, 1,4-dioxane or the like), or a halogenated hydrocarbon (dichlorom ethane, dichloroethane or the like) can be employed, and either continuous polymerization or batch polymerization is possible. [0091] A polymerization temperature is usually in a range of-80°C to 150°C, particularly in a range of-30°C to 100°C. In general, a reaction time is determined appropriately depending on the kind of the intended polymer, and a reactor, and for example, a time in a range of 1 second to 24 hours can be adopted.
[0092] Preferably, the polymerization reaction is performed under an atmosphere of an inert gas such as nitrogen or argon. It is important for the efficient preparation of a polymer that the inert gas and an alkylene oxide are sufficiently dried so as to be free from water. [0093] The resultant alkylene oxide polymer contains a metal catalytic component. However, when a polymerization degree is high, it is not

necessary to remove the metal catalytic component since the content of the
contained metal catalytic component is relatively small. When the removal
of the metal catalytic component is necessary, the alkylene oxide polymer as
produced is washed with water or dilute hydrochloric acid to remove the
metal catalytic component, followed by drying, to obtain an alkylene oxide
polymer.
[0094] The resultant alkylene oxide polymer can be used as a film, a fiber,
an expanded sheet or various molded articles.
[0095] [Process for producing (meth)acrylate ester polymer]
Examples of the (meth)acrylate ester used in the present invention include methacrylate esters such as methyl methacrylate, ethyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, tert-butyl methacrylate, cyclohexyl methacrylate, isobutyl methacrylate, benzyl methacrylate, allyl methacrylate, and isobornyl methacrylate'. and acrylate esters such as methyl acrylate, ethyl acrylate, isopropyl acrylate, n-butyl acrylate, and tert-butyl acrylate.
[0096] These (meth)acrylate esters may be polymerized alone, while a mixture of two or more (meth)acrylate esters may be copolymerized. A method of copolymerizing two or more (meth) acrylate esters is not particularly limited, and examples thereof include a method of initiating polymerization under such a condition that two or more (meth) acrylate esters are present simultaneously, to obtain a random copolymer, and a method of polymerizing the first (meth)acrylate ester in advance, and then adding the second or subsequent (meth)acrylate ester(s) to obtain a block copolymer.
[0097] Amethod of initiating polymerization is not particularly limited. For example, a (meth)acrylate ester is added to the solution of the rare earth metal complex (l) to initiate polymerization, or the rare earth metal complex

(l) is added to the solution of a (meth)acrylate ester to initiate polymerization.
[0098] The polymerization method is not particularly limited, and for example, solution polymerization or slurry polymerization using an aliphatic hydrocarbon (butane, pentane, hexane, heptane, octane or the like), an aromatic hydrocarbon (benzene, toluene or the like), an ether (diethyl ether, tetrahydrofuran, 1,4-dioxane or the like), or a halogenated hydrocarbon (dichlorom ethane, dichloroethane or the like) as a solvent can be employed, and either continuous polymerization or batch polymerization can be employed.
[0099] A polymerization temperature is usually in a range of-80°C to 150°C, particularly preferably in a range of -30°C to 100°C. In general, a polymerization time is determined appropriately depending on the kind of the intended polymer, and a reactor and. for example, a time in a range of 1 second to 24 hours can be adopted.
[0100] Preferably, the polymerization reaction is performed under an atmosphere of an inert gas such as nitrogen or argon. It is important for the efficient preparation of a polymer that the inert gas and a (meth)acrylate ester monomer are sufficiently dried so as to be free from water. [0101] The resultant (meth)acrylate ester polymer contains a metal catalytic component. However, when a polymerization degree is high, it is not necessary to remove the metal catalytic component since the content of the contained metal catalytic component is relatively small. When the removal of the metal catalytic component is necessary, the (meth)acrylate ester polymer as produced is washed with water or dilute hydrochloric acid to remove the metal catalytic component, followed by drying, to obtain the (meth)acrylate ester polymer. [0102] The resultant (meth)acrylate ester polymer can be used as a film, a

fiber, an expanded sheet or various molded articles. Alternatively, the resultant (meth)acrylate ester polymer can be used as an additive for other polymers.
EXAMPLES
[0103] The following examples illustrate the present invention in more detail, but they do not limit the present invention in any way. [0104] ^Production of rare earth metal complex >
Physical properties were measured by the following methods.
(1) Proton nuclear magnetic resonance spectrum ('H-NMR)
Apparatus: EX270 manufactured by JEOL Ltd., or DPX-300 manufactured
by Bruker
Sample cell: 5 mm tube
Measurement solvent: CDCI3 or toluene-ds
Sample concentration: 10 mg/0.5 mL (CDCI3 or toluene-ds)
Measurement temperature: room temperature (about 25°C)
Measurement parameters-' 5 mm probe, MENUFNON, OBNUC 2H,
Accumulation times 16
Pulse angle: 45 degrees
Repetition time: ACQTM 3 seconds, PD 4 seconds
Internal standard: CDCL (7.26 ppm), toluene-ds (2.09 ppm)
(2) Carbon nuclear magnetic resonance spectrum (13C"NMR)
Apparatus: EX270 manufactured by JEOLLtd., or DPX-300 manufactured
by Bruker
Sample cell: 5 rnm4> tube
Measurement solvent: CDCI3 or toluene-dg
Sample concentration: 30 mg/0.5 mL (CDCLs or toluene-ds)
Measurement temperature-' room temperature (about 25°C)

Measurement parameter: 5 mm probe, MENUF NON, OBNUC l3C, accumulation times 256 Pulse angle: 45 degrees
Repetition time-'ACQTM l.S seconds, PD 1.2 seconds Internal standard: CDCI3 (77.47, 77.00, 76.53 ppm) [0105]
(3) Mass spectrum
[Electron ionization mass spectroscopy (EI-MS)] Apparatus: JMS-T100GC manufactured by JEOL Ltd. Ionization voltage: 70 eV Ion source temperature: 230°C Acceleration voltage: 7 kV Mass range: m/z 35-1000 [0106] Example 1
Synthesis of (2-methoxy-3-tert-butyl'5'methylphenyl)chlorodiethylsilane Under nitrogen atmosphere, 2-methodxy-l-bromo-3-tert-butyl-5-methylbenzene (20.00 g, 77.77 mmol) was dissolved in 200 mL of diethyl ether. A 1.57 M hexane solution of n-butyllithium (59.44 mL, 93.32 mmol) was dropwise added at -50DC or lower, and a temperature was raised to room temperature, followed by stirring for 1 hour. All the amount of diethyldichlorosilane (24.44 g, 155.54 mmol) was added to the mixture at once at -50°C or lower, and a temperature was gradually raised to room temperature. After being refluxed for 1 hour, the solution was concentrated under reduced pressure. Hexane was added, the insolubles were filtered off with a Celite filter, and the filtrate was concentrated under reduced pressure. Concentration was further continued at 70°C under reduced pressure for 3 hours to obtain (2-methoxy-3-tert-butyl-5-methylphenyl)chlorodiethylsilane. Resultant (2-methoxy-3-tert-butyl-5-methylphenyl)chlorodiethylsilane was

used in a subsequent reaction without further purification.
■H-NMR (CDCls, 5(ppm»: 1.04-1.17 (m, 10H), 1.39 (s, 9H), 2.32 (s, 3H), 3.75
(s, 3H), 7.24 (s, lH),7.3l(s, 1H)
13C-NMR (CDCI3, 5(ppm)): 6.96, 9.29, 21.07, 31.37, 35.07, 64.20, 127.41,
131.58, 132.72, 135.51, 141.89, 162.92
[0107] Example 2
Synthesis of (2methoxy-3"tertbutyl-5-methylphenyl)(2,3,4,5-tetramethyl-
cyclopentadien- l-yl)diethylsilane
Under nitrogen atmosphere, 76 mL of THF was added to sodium hydride (60 wt%, 1.14 g, 47.42 mmol). Atemperature of the tetrahydrofuran slurry of sodium hydride was raised to 50°C. Aniline (0.29 g, 3.16 mmol) was added, and the mixture was further stirred at 50°C for 1 hour. A solution of 1,2,3,4-tetramethylcyclopentadiene (4.25 g, 34.78 mmol) in 19 mL of THF was slowly dropwise added thereto. After the completion of addition, the mixture was further stirred at 50°C for 3 hours until the generation of a hydrogen gas ceased. After cooled to 20°C, a solution of (2-methoxy-3'tert-butyl-5-metliylphenyl)chlorodiethylsilane (9.45 g, 31.61 mmol) in 19 mL of toluene was dropwise added, and stirring was continued at room temperature for 3 hours. The resultant reaction solution was dropwise added to a mixed solution obtained by cooling 47 mL of a 10% aqueous sodium bicarbonate solution and 47 mL of a 10% aqueous sodium carbonate solution at 0°C to terminate the reaction, 47 mL of toluene was added, and the mixed solution was separated. After drying with sodium sulfate, concentration of the solution under reduced pressure afforded a mixture of
(2-methoxy3-tert-butyl-5-methylphenyl)(2;3,4,5-tetraniethylcyclopentadien-l-yl)diethylsilane. (2-Methoxy-3-tert-butyl-5-methylphenyl)-(2.3,4,5-tetramethylcyclopentadien-l-yl)diethylsilane was purified by silica

gel column chromatography.
^■NMR (toluene-ds, 5 (ppm)): 0.96-1.00 (m, 10H), 1.44 (s, 9H), 1.81 (s, 6H),
1.84 (s, 6H), 2.20 (s, 3H), 3.46 (s, 1H), 3.58 (s, 3H), 7.11 (s, 1H), 7.18 (s, 1H)
I3C-NMR (toluene-ds, 5 (ppm)): 4.62, 8.38, 11.38, 14.62, 21.21, 30.31, 31.41,
35.22, 129.92, 130.11, 131.91, 133.72, 135.90, 135.94, 141.88, 164.14
[0108] Example 3
Synthesis of [l-(diethyl{2-methoxy-3'tert-butyl-5-methylphenylisilyl)'
2,3,4,5-tetramethylcyclopentamenyl]bis(o-N,N-dimethylaminobenzyl)-
scandium (hereinafter, referred to as scandium complex (l))

Tris(o-N,N-dimethylaminobenzyl)scandium was synthesized according to the published article (J. Am. Chem. Soc. 1978, 100, 8068). ■H-NMR (toluene-ds, 5 (ppm)): 1.58 (s, 6H), 2.28 (s, 18H), 6.71-6.78 (m, 6H), 6.85-6.95 (m, 6H)
Mass spectrum (EI-MS, m/z): 313 (M+-134), 268, 134, 91, 65
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyi)-scandium (0.50 g, 1.12 mmol) was dissolved in 6 mL of THF, and a mixture prepared by dissolving (2-methoxy-3-tert-butyl-5-methylphenyl)-(2,3,4,5-tetramethylcylcopentadien-l-yl)diethylsilane (0.43 g, 1.12 mmol) in 6 mL of tetrahydrofuran was added at room temperature. Stirring was continued at room temperature for 3 days. The mixture was concentrated under reduced pressure, and hexane was added to obtain scandium complex (1)(0.48 g, yield 61.4%) as a pale yellow solid.
'H-NMR (toluene-ds, 5 (ppm)): 1.22-1.70 (m, 10H), 1.40 (s, 9H), 1.54(s. 4H), 1.73 (s, 6H), 1.76 (s, 6H), 2.30 (s, 3H). 2.39 (s, 12H), 2.84 (s, 3H). 6.71-6.83 (m, 4H). 6.93-7.12 (m. 4H). 7.18 (s, 1H). 7.39 (s, 1H) Mass spectrum (EI-MS, m/z): 384 (M+-313), 355. 325. 235, 207, 177. 161, 117.

57
[0109] Example 4
Synthesis of [l-(diethyl{2-methoxy-3-tert-butyl-5-methyphenyl}silyl)-
2;3,4,5-tetramethylcyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)-
lutetium (hereinafter, referred to as lutetium complex (l))
^Synthesis of tris(o-N,Ndimethylaminobenzyl)lutetiura>
Tris(o-N,N-dimethylaminobenzyl)lutetium was synthesized in the same manner as that for the synthesis of tris(o-N,N-dimethylaminobenzyl)-scandium in Example 3 except that lutetium chloride was used. !H-NMR (toluene-ds, 6 (ppm)): 1.41 (s, 6H), 2.18 (s, 18H), 6.65-6.78 (m, 6H), 6.91-7.07 (m, 6H)
Mass spectrum (EI-MS, m/z): 443 (M+-134), 268, 134, 120, 118, 91, 65
Under nitrogen atmosphere, tris(o-N,Ndimethylaminobenzyl)-lutetium (0.50 g, 1.04 mmol) was dissolved in 6 mL of tetrahyhdrofuran, and a mixture prepared by dissolving (2-methoxy-3-tert-butyl-5-methylphenyl)-(2,3,4,5-tetramethylcyclopentadien-lyl)diethylsilane (0.40 g, 1.04 mmol) in 6 mL of tetrahydrofuran was added at room temperature. Stirring was continued at room temperature for 3 days, and the mixture was stirred at 60°C for 6 hours. The mixture was concentrated under reduced pressure, andhexane was added to obtain lutetium complex (l) (0.51 g, yield 59.2%) as a white solid.
LH-NMR (toluene-ds, 5 (ppm)): 1.23-1.65 (m, 10H), 1.35 (s, 4H), 1.40(s, 9H), 1.83 (s, 12H), 2.27 (s, 3H), 2.32 (s, 12H), 2.88 (s, 3H), 6.66-6.80 (m, 4H), 6.94-7.15 (m, 4H), 7.19 (s, 1H). 7.43 (s, 1H)
Mass spectrum (EI-MS, m/z): 384 (M+- 443), 355, 325, 263, 235, 207, 179, 135. 120.89,57 [0110] Example 5

Synthesis of [l-{l-(2-methoxy-3-tert-butyI-5-methylphenyl)-l-methylethyl}' cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)yttrium (hereinafter, referred to as yttrium complex (l)) ^Synthesis of tris(o-N,N-dimethylaminobenzyl)yttrium>
Tris(o-N,N-dimethylaminobenzyl)yttrium was synthesized in the same manner as that for the synthesis of tris(o-N.N-dimethylaminobenzyl)-scandium in Example 3 except that yttrium chloride was used. JH-NMR (toluene-ds, 8 (ppm))-' 1.54 (s, 6H), 2.11 (s, 1SH), 6.58-6.66 (m, 3H), S.80-6.82 (m, 3H), 6.90-7.03 (m, 6H)
Mass spectrum OEI-MS, m/z): 357 (M+-134), 268, 134, 120, 91, 65
6Tert-butyl-2-[l-(cyclopentadienyl)-l-methylethyl]-l-methoxy-4-methylbenzene was synthesized according to the publication (JP-A-09-87313).
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)-yttrium (0.50 g, 1.02 mmol) was dissolved in 5 mL of tetrahydrofuran. and a mixture prepared by dissolving 6-tert-butyl-2[l-(cyclopentadienyl)-l~ methylethyl]-l-methoxy-4-methylbenzene (0.29 g, 1.02 mmol) in 5 mLof tetrahydrofuran was added at room temperature. After stirring was continued at room temperature for 24 hours, the mixture was concentrated under reduced pressure, and pentane was added to obtain yttrium complex (1) (0.34 g, yield 52.4%) as a white solid.
iH-NMR (toluene-ds, 5 (ppm)): 1.45 (s. 13H), 1.90 (s, 6H), 2.25 (s, 15H). 3.01 (s, 3H). 5.58 (br s, 2H), 5.71-5.75 (m, 2H), 6.66-6.78 (m. 4H), 6.91-7.04 (m, 4H). 7.10 (brs, 2H) Mass spectrum (EI-MS, m/z): 640 CM")

[0111] Example 6
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyU-
cyclopentadienyl]bis(o-N,N-dimethylammobenzyl)scandium (hereinafter,
referred to as scandium complex (2))

Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)scandium (0.50 g, 1.12 mmol) was dissolved in 6 mL of tetrahydrofuran, and a mixture prepared by dissolving 6tert-butyl-2-[l(cyclopentadienyl)-l-methylethyl]-l-methoxy-4-methyl-benzene (0.32 g, 1.12 mmol) in 6 mL of tetrahydrofuran was added at room temperature. After stirring was continued at room temperature for 24 hours, the mixture was concentrated under reduced pressure, and pentane was added, followed by cooling to -20°C. The insolubles were filtered off, and the filtrate was cooled to - 20°C. The resultant precipitate was washed with cold pentane to obtain scandium complex (2) (0.25 g, yield 37.3%) as a pale yellow solid.
iH-NMR (toluene-ds, 6 (ppm))- 1.44 (s, 13H), 1.82 (s, 6H), 2.22 (s, 3H), 2.37 (s, 12H), 3.00 (s, 3H), 5.60 (br s, 2H), 5.70 (br s, 2H), 6.69-6.71 (m, 2H), 6.81-6.84 (m, 2H), 6.95-7.00 (m, 4H), 7.07-7.10 (m, 2H) Mass spectrum (EI-MS, m/z): 596 (M+) [0112] Example 7
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyl}-cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)lutetium (hereinafter, referred to as lutetium complex (2))
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)-lutetium (0.70 g. 1.21 mmol) was dissolved in 6 mL of tetrahydrofuran, and a mixture prepared by dissolving 6-tert-butyl-2-[l-(cyclopentadienyl)-l-

methylethylM-methoxy-4-methyl'benzene (0.34 g, 1.21 mmol) in 6 mL of
tetrahydrofuran was added at room temperature. After stirring was
continued at room temperature for 24 hours, the mixture was concentrated
under reduced pressure, and pentane was added, followed by cooling to '20°C.
The resultant precipitate was washed with cold pentane to obtain lutetium
complex (2) (0.62 g, yield 70.5%) as a white solid.
'H-NMR (toluene-dg, 5 (ppm)): 1.45 (s, 13H), 1.60-2.10 (br d, 6H), 2.24 (s, 3H),
2.20-2.47 (br s, 12H), 3.01 (s, 3H), 5.40-5.80 (br, 4H), 6.65-6.68 (m, 2H),
6.76-6.82 (m, 2H), 6.92-7.01 (m, 4H), 7.07-7.12 (m, 2H)
Mass spectrum (EI-MS, m/z): 726 (M+)
[0113] Example 8
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyl}-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)thuhum (hereinafter,
referred to as thulium complex (l))

Tjris(o-N,N-dimethylaminobenzyl)thuhum was synthesized in the same manner as that for the synthesis of tris(oN,N-dim ethyl amin oh enzyl)-scandium in Example 3 except that thulium chloride was used. Mass spectrum (EI-MS, m/z): 571 (M+), 437, 134, 120, 91, 65
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)-thulium (0.70 g, 1.22 mmol) was dissolved in 6 mL of tetrahydrofuran, and a mixture prepared by dissolving 6-tert-butyl-2-[l-(cyclopentadienyl)-l-methylethyl]-l-methoxy-4-methylbenzene (0.35 g, 1.22 mmol) in 6 mL of tetrahydrofuran was added at room temperature. After stirring was continued at room temperature for 24 hours, the mixture was concentrated under reduced pressure, and pentane was added, followed by cooling to -20°C. The resultant precipitate was washed with cold pentane to obtain thulium

complex (1) (0.63 g, yield 71.8%) as a yellow solid.
Mass spectrum (EI-MS, m/z): 720 (M+)
[0114] Example 9
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyl}-
cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)erbium (hereinafter,
referred to as erbium complex (l))

Tris(o-N,N-dimethylaminobenzyl)erbium was synthesized in the same manner as that for the synthesis of tris(o-N,N-dimethylaminobenzyl)-scandium in Example 3 except that erbium chloride was used. Mass spectrum (EI-MS, m/z): 568 (M+), 434, 134, 120, 91, 65
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)-erbium (0.70 g, 1.23 mmol) was dissolved in 6 mL of tetrahydrofuran, and a mixture prepared by dissolving 6-tert-butyl-2-[r(cyclopentadienyl)-l-methylethyl]-lmethoxy-4-methylbenzene (0.35 g, 1.23 mmol) in 6 mL of tetrahydrofuran was added at room temperature. After stirring was continued at room temperature for 24-hours, the mixture was concentrated under reduced pressure, and pentane was added, followed by cooling to -20°C. The resultant precipitate was washed with cold pentane to obtain erbium complex (l) (0.65 g, yield 74.1%) as a pale pink solid. Mass spectrum (ELMS, m/z)'- 719 (M+) [0115] Example 10
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyl}-cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)holmium (hereinafter, referred to as holmium complex (l))
Tris(o-N.N-dimethylaminobenzyl)holmium was synthesized in the

same manner as that for the synthesis of tris(o-N,N-dimethylaminobenzyl)-scandium in Example 3 except that holmium chloride was used. Mass spectrum (EI-MS, m/z): 567 (M+), 433. 135, 120, 91, 65
Under nitrogen atmosphere, tris(o-N,N-dimethylamiiiobenzyl)-holmium (0.70 g, 1.23 mmol) was dissolved in 6 mL of tetrahydrofuran, and a mixture prepared by dissolving 6-tert-butyl-2-[l-(cyclopentadienyl)-l-methylethyl]-l-methoxy-4-rnethylbenzene (0.35 g, 1.23 mmol) in 6 mL of tetrahydrofuran was added at room temperature. After stirring was continued at room temperature for 24 hours, the mixture was concentrated under reduced pressure, and pentane was added, followed by cooling to -20°C. The resultant precipitate was washed with cold pentane to obtain holmium complex (l) (0.61 g, yield 69.7%) as a pale orange solid. Mass spectrum (EI-MS, m/z): 716 (M+) [0116] Example 11
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5methylphenyl)-l'methylethyl}-cyclopentadienyl]bis(o-N,N-dimethylaminobenzyl)dysprosium (hereinafter, referred to as dysprosium complex (l))
Tris(o-N,N- dim ethyl aminobenzyl) dysprosium was synthesized in the same manner as that for the synthesis of tris(o-N,N-dimethylaminobenzyl)-scandium in Example 3 except that dysprosium chloride was used. Mass spectrum (EI-MS, m/z)- 432 (M+-133>, 268, 135, 120, 65
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)-dysprosium (0.70 g, 1.24 mmol) was dissolved in 6 mL of tetrahydrofuran. and a mixture prepared by dissolving 6-tert-butyl-2-[l-(cyelopentadienyl)-1-methylethyli-l-methoxy-4-methylbenzene (0.35 g. 1.24 mmol) in 6 mL of

tetrahydrofuran was added at room temperature. After stirring was
continued at room temperature for 24 hours, the mixture was concentrated
under reduced pressure, and pentane was added, followed by cooling to -20
°C. The resultant precipitate was washed with cold pentane to obtain
dysprosium complex (l) (0.63 g, yield 71.6%) as a pale yellow solid.
Mass spectrum (EI-MS, m/z): 714 (M+)
[0117] Example 12
Synthesis of [l-{l-(2-methoxy-3-tert-butyl-5-methylphenyl)-l-methylethyl}-
cyclopentadienyl]bis(o-N,N"dimethylaminobenzyl)terbium (hereinafter,
referred to as terbium complex (l))

Tris(o-N,N-comethylaminobenzyl)terbium was synthesized in the same manner as that for the synthesis of tris(o-N,N-dimethylaminobenzyl)-scandium in Example 3 except that dysprosium chloride was used. Mass spectrum (EI-MS, m/z): 427 (M+-134), 268, 135, 120, 91, 65
Under nitrogen atmosphere, tris(o-N,N-dimethylaminobenzyl)-terbium (0.70 g, 1.25 mmol) was dissolved in 6 mL of tetrahydrofuran, and a mixture prepared by dissolving 6-tertbutyl-2-[l-(cyclopentadienyl)-l-methylethyl]-l-methoxy-4-methylbenzene (0.35 g, 1.25 mmol) in 6 mL of tetrahydrofuran was added at room temperature. After stirring was continued at room temperature for 24 hours, the mixture was concentrated under reduced pressure, and pentane was added to remove the insolubles by filtration. The filtrate was cooled to -20°C. The resultant precipitate was washed with cold pentane to obtain terbium complex (l) (0.56 g, yield 62.5%) as a yellow sohd.
Mass spectrum (ELMS. m/zV- 710 (M+) [0118]

Physical properties were measured by the following method. [0119] (1) 1-Hexene unit content in copolymer (SCB, unit: 1/1000C)
Using an infraied spectrophotometer (EQUINOX 55 manufactured by Brulcer), the unit content was obtained by infrared spectroscopy. The characteristic absorption of butyl branches was expressed using a peak in a range of 1378 cm'1 to 1303 cm'1, and a 1-hexene unit content was expressed as the number of butyl branches per 1000 carbon atoms of an ethylene-1-hexene copolymer. [0120] (2) Molecular weight and molecular weight distribution
A molecular weight and a molecular weight distribution were measured by gel permeation chromatography (GPC) under the following conditions. The molecular weight distribution was assessed by a ratio (Mw/Mu) of a weight average molecular weight (Mw) to a number average molecular weight (Mn).
Apparatus^ Pump apparatus (LC pump) Model 305 (pump head 25.SC) manufactured by Gilson
Column: PLgel Mixed-B 10 urn (7.5 mmcf> x 300 mm) manufactured by Polymer Laboratories Measurement temperature- 160°C Mobile phase: Orthodichlorobenzene
Sample concentration: Copolymer 1 mg/l,2,4-trichlorobenzene 1 mL Flow rate: 2 mL/min.
Standard materials: (Standard polystyrene molecular weight) 5,000, 10,050, 28.500, 65,500, 185,400, 483,000, 1,013,000, 3,390,000 [0121] Ethylene and 1-hexene was copolymerized in the presence of scandium complex (l) obtained in Example 3 as a catalytic component for olefin polymerization using PPR (equipped with 48 autoclaves) manufactured by Symyx under the polymerization conditions described

below.
[0122] Example 13
Under nitrogen atmosphere, 5.0 mL of toluene and 60 y.L of 1-hexene were charged in an autoclave and stabilized at 40°C. Then, ethylene was pressurised to 0.60 MPa and stabilized. To this mixture, 100 p.mol (in terms of Al atoms) of aluminoxane (MMAO manufactured by Tosoh Finechem Corporation, 5.8 wt% Al) and 0.10 ^imol of scandium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer having a molecular weight (Mw) of 676,000, a molecular weight distribution (Mw/Mn) of 11.2, a 1-hexene unit content in a copolymer (SCB) of 10 was produced at a rate 1.9 x 106 g per 1 mol of a catalyst per 1 hour. 10123] Example 14
Polymerization was performed in the same manner as in Example 13 except that the amount of 1-hexene was changed to 50 uL, and a polymerization temperature was changed to 70°C, to produce a polymer having a molecular weight (Mw) of 262,000, a molecular weight distribution (Mw/Mn) of 9.0, and a 1-hexene content in a copolymer (SCB) of 8 at a rate of 6.9 x 10s g per 1 mol of a catalyst per 1 hour. [0124] Example 15
Polymerization was performed in the same manner as in Example 13 except that the amount of 1-hexene was changed to 40 uL, a polymerization temperature was changed to 130°C, and the amount of aluminoxane was changed to 10 (imol, to produce a polymer having a molecular weight (Mw) of 59,000, a molecular weight distribution (Mw/Mn) of 1.6. and a 1-hexene content in a copolymer (SCB) of 1 at a rate of 20.5 x 10G g per 1 mol of a catalyst per 1 hour. [0125] Example 16

Under nitrogen atmosphere, 5.0 mL of toluene and 60 pL of 1-hexene were charged in an autoclave and stabilized at 40°C. Then, ethylene was pressurized to 0.60 MPa and stabihzed. To this mixture, 40 \iL of a hexane solution of triisobutylaluminum (hereinafter, referred to as TIBA (manufactured by Kanto Chemical Co., Inc., TIBA concentration 1.0 mol/L), 0.30 umol of tris(pentafl.uorophenyl)borane, and 0.10 pmol of scandium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer having a molecular weight (Mw) of 1,867,000, a molecular weight distribution (Mw/Mn) of 1.8, and a 1-hexene content in a copolymer (SCB) of 6 was produced at a rate of 1.5 x 10G g per 1 mol of a catalyst per 1 hour. [0126] Example 17
Under nitrogen atmosphere, 5.0 mL of toluene and 60 uX of 1-hexene were charged in an autoclave and stabilized at 40°C. Then, ethylene was pressurized to 0.60 MPa and stabihzed. To this mixture, 40 uL of a hexane solution of TIBA (manufactured by Kanto Chemical Co., Inc., TIBA concentration 1.0 mol/L), 0.30 [unol of dimethylanilinium tetrakis(pentafluorophenyl)borate, and 0.10 nmol of scandium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer having a molecular weight (Mw) of 144,000, a molecular weight distribution (Mw/Mn) of 1.8, and a 1-hexene content in a copolymer (SCB) of 1 was produced at a rate of 44.2 x ioe g per 1 mol of a catalyst per 1 hour. [0127] Example 18
Polymerization was performed in the same manner as in Example 17 except that the amount of 1-hexene was changed to 50 \iL, and a polymerization temperature was changed to 70°C, to produce a polymer having a molecular weight (Mw) of 54,000, a molecular weight distribution

(Mw/Mn) of 1.7, and a 1-hexene content in a copolymer (SCB) of 30 at a rate of 205.0 x i0e g per 1 mol of a catalyst per 1 hour. [0128] Example 19
Polymerization was performed in the same manner as in Example 17 except that the amount of 1-hexene was changed to 40 uL, a polymerization temperature was changed to 130°C, and the amount of a hexane solution of TIBA was changed to 4 uL, to produce a polymer at a rate of 2.7 x 10G g per 1 mol of a catalyst per 1 hour. [0129] Example 20
Under nitrogen atmosphere, 5.0 mL of toluene and 60 uL of 1-hexene were charged in an autoclave and stabilized at 40°C. Then, ethylene was pressurized to 0.60 MPa and stabilized. To this mixture, 40 \xL of a hexane solution of TIBA (manufactured by Kanto Chemical Co., Inc., TIBA concentration 1.0 mol/L), 0.30 umol of triphenylmethyl tetrakis(pentafluorophenyl)borate, and 0.10 umol of scandium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer having a molecular weight (Mw) of 230,000, a molecular weight distribution (Mw/Mn) of 1.9, and a 1-hexene content in a copolymer (SCB) of 5 was produced at a rate of 87.6 x 10G g per 1 mol of a catalyst per 1 hour. [0130] Example 21
Polymerization was performed in the same manner as in Example 20 except that the amount of 1-hexene was changed to 50 uL, and a polymerization temperature was changed to 70°C, to produce a polymer having a molecular weight (Mw) of 98,000, a molecular weight distribution (Mw/Mn) of 1.7, and a 1-hexene content in a copolymer (SCB) of 36 at a rate of 175.3 x 106 gper 1 mol of a catalyst per 1 hour. [0131] Example 22

Polymerization was performed in the same manner as in Example 20 except that the amount of 1-hexene was changed to 40 uL, a polymerization temperature was changed to 130°C, and the amount of a hexane solution of TIBAwas changed to 4 \xL, to produce a polymer at a rate of 1.4 x 106 gper 1 mol of a catalyst per 1 hour. [0132] Example 23
Under nitrogen atmosphere, 5.0 mL of toluene and 50 uL of 1-hexene were charged in an autoclave and stabilized at 70°C. Then, ethylene was pressurized to 0.60 MPa and stabilized. To this mixture, 0.30 umol of triphenylmethyl tetrakis(pentafluorophenyDborate, and 0.10 umol of scandium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer having a molecular weight (Mw) of 1,527,000, a molecular weight distribution (Mw/Mn) of 1.4, and a 1-hexene content in a copolymer (SCB) of 199 was produced at a rate of 14.5 x 106 g per 1 mol of a catalyst per 1 hour. [0133]
Ethylene was homopolymerized in the presence of scandium complex (l) obtained in Example 3 as a catalytic component for olefin polymerization using PPR (equipped with 48 autoclaves) manufactured by Symyx, under the polymerization conditions described below. [0134] Example 24
Under nitrogen atmosphere, 5.0 mL of toluene was charged in an autoclave and stabilized at 40°C. Then, ethylene was pressurized to 0.60 MPa and stabilized. To this mixture, 100 umol (in terms of Al atom) of aluminoxane (MMAO manufactured by Tosoh Finechem Corporation, 5.8 wt% Al), and 0.10 umol of scandium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer was produced at a rate of 1.3 * 105 gper 1 mol of a

catalyst per 1 hour. [0135] Example 25
Polymerization was performed in the same manner as in Example 24 except that 40 uL of a hexane solution of TIBA (manufactured by Kanto Chemical Co., Inc., TIB A concentration 1.0 mol/L) and 0.30 umol of tris(pentafluorophenyl)borane were used in place of methylaluminoxane. As the result of polymerization, a polymer was produced at a rate of 1.1 x 105 g per 1 mol of a catalyst per 1 hour. [0136] Example 26
Polymerization was performed in the same manner as in Example 24 except that 40 uL of a hexane solution of TIBA (manufactured by Kanto Chemical Co., Inc., TIBA concentration 1.0 mol/L) and 0.30 umol of dimethylanilinium tetrakis(pentafluorophenyl)borate were used in place of methylaluminoxane. As the result of polymerization, a polymer was produced at a rate of 24.2 x 106 g per 1 mol of a catalyst per 1 hour. [0137] Example 27
Polymerization was performed in the same manner as in Example 24 except that 40 uL of a hexane solution of TIBA (manufactured by Kanto Chemical Co., Inc., TIBA concentration 1.0 mol/L) and 0.30 umol of triphenylmethyl tetrakis(penta£Luorophenyl)borate were used in place of methylaluminoxane. As the result of polymerization, a polymer was produced at a rate of 30.3 x 106 g per 1 mol of a catalyst per 1 hour. [0138] Example 28
Polymerization was performed in the same manner as in Example 24 except that 0.30 \nn.o\ of triphenyhnethyl tetrakis(pentafluorophenyl)borate was used in place of methylaluminoxane. As the result of polymerization, a polymer was produced at a rate of 9.0 x JO5 g per 1 mol of a catalyst per 1 hour.

[0139] Ethylene and 1-hexene were copolymerized in the presence of
lutetium complex (l) obtained in Example 4 as a catalytic component for
olefin polymerization using PPR (equipped with 48 autoclaves)
manufactured by Symyx under the polymerization conditions described
below.
[01401 Example 29
Under nitrogen atmosphere, 5.0 mL of toluene and 50 uL of 1-hexene were charged in an autoclave and stabilized at 70°C. Then, ethylene was pressurized to 0.60 MPa and stabilized. To this mixture, were added 40 uL of a hexane solution of TIBA (manufactured by Kanto Chemical Co., Inc., TIB A concentration 1.0 mol/L), 0.30 |omol of dimethylanilinium tetrakis(pentafluorophenyl)borate, and 0.10 umol of lutetium complex (l) were added, and polymerization was performed for 30 minutes. As the result of polymerization, a polymer having a molecular weight (Mw) of 508,000, a molecular weight distribution (Mw/Mn) of 22.7, and a 1-hexene content in a copolymer (SCB) of 49 was produced at a rate of 1.6 x 10s g per 1 mol of a catalyst per 1 hour. [0141]
tO 142] A molecular weight and a molecular weight distribution were measured by gel permeation chromatography (GPC) according to the following method. Apparatus: HLC-8120GPC (RI) Column: TSKgel, GMH HR-M Flow rate: 0.5 mL/min Measurement temperature: 40°C Mobile phase: THF Standard material: Polystyrene

[0143] Example 30
Under nitrogen atmosphere, all the amount of a toluene solution (2 mL) of scandium complex (2) (37.6 mg, 0.063 mmol) was added at once to e-caprolactone (2.87 g, 25.2 mmol) while vigorously stirring with a magnetic stirrer at room temperature. One (l) minute after addition, methanol (100 mL) was added to terminate polymerization, and the resultant white solid was collected by filtration. Vacuum drying at 60°C afforded polycaprolactone (2.84 g, yield 99%). The resultant polycaprolactone was subjected to GPC analysis to find that a weight average molecular weight Mw (in terms of polystyrene) was 56,700, and a molecular weight distribution Mw/Mn was 1.39. [0144] Example 31
Under nitrogen atmosphere, all the amount of a toluene solution (4 mL) of scandium complex (2) (38.5 mg, 0.065 mmol) was added at once to e-caprolactone (5.75 g, 50.4 mmol) while vigorously stirring with a magnetic stirrer at room temperature. Three (3) minutes after addition, methanol (100 mL) was added to terminate polymerization, and the resultant white solid was collected by filtration. Vacuum drying at 60°C afforded polycaprolactone (5.04 g, yield 88%). The resultant polycaprolactone was subjected to GPC analysis to find that a weight average molecular weight Mw (in terms of polystyrene) was 113,000, and a molecular weight distribution Mw/Mn was 1.58. [0145] Example 32
Under nitrogen atmosphere, all the amount of a toluene solution (2 mL) of scandium complex (l) (43.9 mg, 0.063 mmol) was added at once to e-caprolactone (2.88 g, 25.2 mmol) while vigorously stirring with a magnetic stirrer at room temperature. One (l) minute after addition, methanol (100 mL) was added to terminate polymerization, and the resultant white solid

was collected by filtration. Vacuum drying at 60°C afforded polycaprolactone (2.73 g, yield 95%). The resultant polycaprolactone was subjected to GPC analysis to find that a weight average molecular weight Mw was 49,400, and a molecular weight distribution Mw/Mn was 1.77. [0146] Example 33
Under nitrogen atmosphere, all the amount of a toluene solution (2 mL) of yttrium complex (l) (41.0 mg, 0.064 mmol) was added at once to e-caprolactone (2.87 g, 25.2 mmol) while vigorously stirring with a magnetic stirrer at room temperature. Fifteen (15) seconds after addition, methanol (100 mL) was added to terminate polymerization, and the resultant white solid was collected by filtration. Vacuum drying at 60°C afforded polycaprolactone (2.79 g, yield 97%). The resultant polycaprolactone was subjected to GPC analysis to find that a weight average molecular weight Mw (in terms of polystyrene) was 41,900, and a molecular weight distribution Mw/Mn was 1.88. [0147] Example 34
Under nitrogen atmosphere, all the amount of a toluene solution (2 mL) of lutetium complex (2) (45.8 mg, 0.063 mmol) was added at once to s-caprolactone (2.88 g, 25.2 mmol) while vigorously stirring with a magnetic stirrer at room temperature. Ten (10) seconds after addition, methanol (100 mL) was added to terminate polymerization, and the resultant white solid was collected by filtration. Vacuum drying at 60°C afforded polycaprolactone (2.79 g, yield 97%). The resultant polycaprolactone was subjected to GPC analysis to find that a weight average molecular weight Mw (in terms of polystyrene) was 57,700. and a molecular weight distribution Mw/Mn was 2.23. [0148]
A molecular weight and a molecular weight distribution were

measured by gel permeation chromatography (GPC) according to the
following method.
Apparatus: HLO8120GPC (RI)
Column'- TSKgel, GMH HR-M
Flow rate: 0.5 mL/min
Measurement temperature: 40°C
Mobile phase: THF
Standard material: Polystyrene
Polymerization of cyclohexene oxide
[0149] Example 35
Under nitrogen atmosphere, scandium complex (2) (44.3 mg, 0.06 mmol) was added to cyclohexene oxide (2.47 g, 25.20 mmol) while stirring at room temperature to thereby initiate polymerization. Polymerization was performed at room temperature for 30 minutes, and methanol (100 mL) was added to terminate polymerization, and a polymer was obtained by filtration. The resultant polymer was vacuum-dried (50DC, 3 hours) to obtain poly (cyclohexene oxide) as a white solid (1.64 g, yield 66%). The resultant poly (cyclohexene oxide) had a weight average molecular weight Mw (in terms of polystyrene) of 495,000, and an Mw/Mn of 2.06. [0150] Example 36
Under nitrogen atmosphere, all the amount of a catalyst solution obtained by dissolving scandium complex (2) (37.6 mg, 0.06 mmol) in toluene (2 mL) was added at once to cyclohexene oxide (2.47 g, 25.20 mmol) while stirring at room temperature to thereby initiate polymerization. Polymerization was performed at room temperature for 6 hours, methanol (100 mL) was added to terminate polymerization, and a polymer was obtained by filtration. The resultant polymer was vacuum-dried (60°C. 3 hours) to obtain poly (cyclohexene oxide) as a white solid (0.34 g, yield 14%).

The resultant poly(cyclohexene oxide) had a weight average molecular weight Mw (in terms of polystyrene) of 436,000, and an Mw/Mn of 2.01. [0151] Example 37
Under nitrogen atmosphere, all the amount of a catalyst solution obtained by dissolving scandium complex (l) (37.6 mg, 0.06 mmol) in toluene (2 raL) was added at once to cyclohexene oxide (2.47 g, 25.20 mmol) while stirring at room temperature to thereby initiate polymerization. Polymerization was performed at room temperature for 6 hours, methanol (100 mL) was added to terminate polymerization, and a polymer was obtained by filtration. The resultant polymer was vacuum-dried (60°C, 3 hours) to obtain poly(cyclohexene oxide) as a white solid (0.21 g, yield 9%). The resultant poly (cyclohexene oxide) had a weight average molecular weight Mw (in terms of polystyrene) of 207,000, and an Mw/Mn of 1.54. [0152] [0153] Tacticity was measured by proton nuclear magnetic resonance spectrum 0H-NMR) according to the published article (e.g. OrganometaUics 2007,26, 187-195).
Apparatus'- EX270 manufactured by JEOLLtd., or DPX-300 manufactured by Bruker
Sample cell; 5 mmc|> tube Measurement solvent: CDCI3 Sample concentration: 30 mg/0.5 mL (CDCI3) Measurement temperature: room temperature (about 25°C) Measurement parameter: 5 mraiji probe, MENUF NON. OBNUC ]H, Accumulation times 16 Pulse angle: 45 degrees
Repetition time- ACQTM 3 seconds, PD 4 seconds Internal standard: CDCI3 (7.26 ppm)

[0154] Example 38

Under nitrogen atmosphere, all the amount of a catalyst solution obtained by dissolving scandium complex (2) (37.6 mg, 0.06 mmol) in toluene (2 mL) was added at once to methyl methacrylate (2.52 g, 25.20 mmol) while stirring at loom temperature to thereby initiate polymerisation. Polymerization was performed at room temperature for 6 hours, methanol (100 mL) was added to terminate polymerization, and a polymer was obtained by filtration. The resultant polymer was vacuum-dried (80CC, 3 hours) to obtain polyGnethyl methacrylate) as a white solid (0.26 g, yield 11%). The resultant polyGnethyl methacrylate) had a weight average molecular weight Mw (in terms of polystyrene) of 72,000, an Mw/Mn of 2.13, and a stereoregularity rr/mr/mm of 73.0/22.8/4.2.




CLAIMS
1. A cover coating composition for a glass lining, comprising a frit constituting the composition, which mainly includes 65 to 75 mol% of Si02, 2 to 8 mol% of Zr02, 10 to 22 rnol% of R20 where R represents Li, K, or Cs, and 2 to 12 mol% of R'O where R' represents Mg, Ca, Sr, or Ba, and the frit is free of Na20.
2. A cover coating composition for a glass lining according to claim 1, wherein the frit includes one or more kinds selected from the group consisting of Ti02, A1203, Laa03, B203, and ZnO.
3. A cover coating composition for a glass lining according to claim 2, wherein a content of Ti02 is in a range of 0.1 to 4 mol%, a content of A1203 is in a range of 0.1 to 4 mol%, a content of La203 is in a range of 0.1 to 4 mol%, a content of B203 is in a range of 0.1 to 4 mol%, and a content of ZnO is in a range of 0.1 to 4 mol%, and in a case where two or more kinds are used in combination, a total amount thereof is in a range of 0.2 to 5 mol%.
4. A cover coating composition for a glass lining according to any one of claims 1 to 3, comprising up to 3 mass% of one or more kinds of coloring components selected from CoO, Sb203, Cr203, Fea03, Sn02, and Ce02 in terms of Fe203 with respect to 100 rnass% of the frit.

5. A cover coating composition for a glass lining according
to any one of claims 1 to 4, wherein up to 5 mol% of each of Si02,
A1203, and CaO components are used in a form of a fluoride.
6. A cover coating composition for a glass lining according
to any one of claims 1 to 5, wherein a linear thermal expansion
coefficient (100 to 400°C) is in a range of 85 to 110xlo"7° C"1.
7. A cover coating composition for a glass lining according
to any one of claims 1 to 6, further comprising 0.01 to 1.5 parts
by mass of a metal fiber having a diameter of 0.1 to 30 pm, a length
of 0.005 to 3 mm, and a shape ratio of the length to the diameter
of 50 or more with respect to 100 parts by mass of the frit.
8. A cover coating composition for a glass lining according
to claim 7, wherein the metal fiber comprises one or more kinds
selected from the group consisting of noble metal-based metals and
alloys of platinum and platinum group metals.


Documents:

http://ipindiaonline.gov.in/patentsearch/GrantedSearch/viewdoc.aspx?id=JXm2u+TBlQm86ff1AUIIPg==&loc=egcICQiyoj82NGgGrC5ChA==


Patent Number 272539
Indian Patent Application Number 684/CHENP/2009
PG Journal Number 15/2016
Publication Date 08-Apr-2016
Grant Date 07-Apr-2016
Date of Filing 05-Feb-2009
Name of Patentee IKEBUKURO HORO KOGYO CO., LTD.
Applicant Address 735 OAZA SHIMOTOMI, TOKOROZAWA-SHI, SAITAMA 359-0001
Inventors:
# Inventor's Name Inventor's Address
1 IIZAWA, YOSHIHIRO, 11-14-103, SASAI 1-CHOME, SAYAMA-SHI, SAITAMA 350-1327,
2 SHIRASAKI, MASAHIRO, SUNNY CREST MANSION 105, 753, KAMIARAI, TOKOROZAWA-SHI, SAITAMA 359-1142,
3 KAWASHIMA, TAKASHI, 2-20-11-210, KOTESASHI-CHO, TOKOROZAWA-SHI, SAITAMA 359-1141
4 MORI, OSAMU, C/O IKEBUKURO HORO KOGYO CO., LTD. 735, OAZA SHIMOTOMI, TOKOROZAWA-SHI, SAITAMA 359-0001
PCT International Classification Number C03C8/02
PCT International Application Number PCT/JP07/65163
PCT International Filing date 2007-08-02
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 2006-214613 2006-08-07 Japan