Title of Invention

A PROCESS FOR REDUCING THE CONCENTRATION OF NITROGEN OXIDES IN COMBUSTION GASES FROM A PLURALITY OF COMBUSTORS

Abstract Disclosed is a system which enables the efficient utilization of urea for selective catalytic reduction (SCR) of NOx by gasifying it and feeding it to a plurality of selective catalytic reduction units associated with a plurality of gas turbines. The invention enables feeding a gasified product of the urea with the ability to fully control separate SCR units without excessive reagent usage or loss of pollution control effectiveness. Controllers determine the amount of reagent required for each turbine to control NOx emissions and then mixes the gasified urea with the correct amount of carrier gas for efficient operation of each separate SCR unit despite the demand variation between the turbines. In this manner the gasification unit can be properly controlled to provide urea on demand without the need for storing large inventories of ammonia-containing gasses to correct for fluctuations in demand.
Full Text United States Patent Application
Selective Catalytic NOx Reduction Process And Control System
Related Application
[000] This application is a continuation of copending US Provisional Application SN 60986917,
filed November 9, 2007, the disclosure of which is incorporated herein in its entirety.
Field of the Invention
[001] The invention relates generally to the efficient utilization of urea for selective catalytic
reduction (SCR) of NOx, and more particularly to feeding a gasified product of the urea to feed
multiple turbine power units from a single unit, which converts urea to ammonia-containing
SCR reagent yet maintains the ability to fully control separate SCR units without excessive
reagent usage or loss of pollution control effectiveness.
Background of the Invention
[002] The use of turbines to generate power is economical in many situations where more
conventional powerplants cannot be contemplated. To their great credit, they generally
operate with minimal generation of NOx and can utilize fuels, such as digester and landfill gases.
However, they do generate regulatory significant amounts of NOx, and efforts are made to
reduce emissions to even lower levels.
[003] Digester and landfill gases are gaseous by-products, principally comprised of methane
and carbon dioxide, of anaerobic decomposition of organic materials from sewage treatment or
landfills. These are not clean fuels according to criteria that utilities normally consider. Trace
quantities of offensive compounds are typically found in the gases and often include hydrogen
sulfide, ammonia and acid gas forming compounds. In addition, some compounds present in
the gas and are known to clog NOx reduction catalysts and shorten the life of the turbines. The
net effect for operators is that utilization of this low-cost fuel can present additional costs in
terms of shortened turbine life, corroded ductwork and fouled catalysts.
[004] Unless these costs can be recovered by taking good advantage of the energy value of
these fuels, the environment will suffer and their energy value will likely be replaced with
imported petroleum. It is, therefore, advantageous that all costs be recovered by the facility
operators, burned in combustion devices such as turbines to either generate electricity or
directly power equipment, and treated by suitable NOx reduction technology, the best of which is
SCR if it can be done effectively without storing dangerous ammonia in a system which is as
flexible as the power grid is to energy demand.
[005] SCR has been proven to be highly effective at NOx reduction, and SCR units can generally
be scaled to the size required for turbines. However, SCR units typically require the use of
ammonia as a reducing reagent, and it is a common problem that ammonia is difficult and
dangerous to store, especially in populated areas. Thus, the use of ammonia generators such as
described in U. S. Patent No. 7,090,810 to Sun, ef a/., and U. S. Patent No. 6,077,491 to Cooper,
et a\., are often required, but their control for multiple turbine units has not been addressed and
can be more costly or difficult than economics may permit in some installations, such as turbines
for use with digester and landfill gases.
[006] The digester and landfill gases, which have more traditionally been burned by a flare
because of the low quality of the gases, can create costs that are difficult to recover. For these
gases, the problem of economics is especially great. Installations requiring more than one turbine
cannot presently benefit from a single urea-based ammonia SCR plant. Unfortunately, it has been
seen that utilization of a single urea conversion unit for each turbine is the most practical
approach.
[007] However, because the demand on the turbines for power fluctuates over time - with
daily and seasonal fluctuations - single ammonia generators have not been practical. SCR units
typically employ ammonia injection grids (AIGs), which are essentially arrays of distribution pipes
with holes arranged through which the ammonia is preferably ejected with a carrier gas to
provide sufficient momentum for the gas at each location and thereby achieve uniform
distribution of ammonia. When demand is low, immediate decrease of ammonia to one SCR unit
for one turbine, will create a temporary excess of ammonia for the others. Without employing
storage tanks, which is to avoided for ammonia safety reasons, there is currently no good way to
accommodate the fluctuations. Distribution will be adversely affected or excess ammonia will be
supplied and result in ammonia slip.
[008] There is a present need for a process, apparatus and system for efficient utilization of
urea for selective catalytic reduction (SCR) of NOx, and more particularly for feeding a gasified
product of the urea to multiple turbine power units from a single urea gasification unit.
[009] There is a particular need for such a system which converts urea to ammonia, yet
maintains the ability to fully control separate SCR units without excessive reagent usage or loss
of pollution control effectiveness.
Summary of the Invention
[010] The present invention provides a process for reducing the concentration of nitrogen
oxides in combustion gases from a plurality of turbines or other combustors, each of which has
an associated selective catalytic NOx reduction catalyst effective for utilizing gasified urea, the
process comprising: heating aqueous urea at conditions of temperature and pressure for a time
effective to gasify the urea and water by mixing the aqueous urea with a heated gas stream in
amounts relative to the amounts of urea and water to produce a first gasified reductant stream
comprising a predetermined mass and concentration of ammonia; monitoring the demand for
urea at each of the plurality of turbines; feeding the first gasified reductant stream to each
turbine at a rate sufficient to supply gasified reductant to supply the monitored demand to the
selective catalytic NOx reduction catalyst associated with each turbine; determining an amount of
carrier gas needed to achieve a predetermined degree of mixing of the gasified reagent with
combustion gases generated at each turbine; based on this determination, admixing a
determined amount of carrier gas with the first gasified reductant stream to provide a catalyst
feed stream associated with each turbine; and at each turbine, introducing an associated catalyst
feed stream by means of an ammonia injection grid to the combustion gases upstream of the
catalyst under conditions effective to reduce the concentration of NOx in the effluent from each
turbine.
[011] The invention also comprises the system and apparatus described and illustrated for
accomplishing the process as described and reasonable variations of it.
Description of the Drawings
[012] The accompanying drawings, which are incorporated in and constitute a part of the
specification, illustrate presently preferred embodiments of the invention, and together with the
general description given above and the detailed description of the preferred embodiments
given below, serve to explain the principles of the invention. As shown throughout the drawings,
like reference numerals designate like or corresponding parts.
[013] Fig. 1 is a schematic flow diagram of a preferred embodiment of the process and system
of the invention.
[014] Fig. 2 is a schematic representation of a single turbine with an SCR unit supplied with
gasified reductant in accord with the invention.
[015] Fig. 3 is a schematic diagram on one form of ammonia injection grid the operation of
which in an SCR system that can be improved according to the invention.
Detailed Description of the Invention
[016] In describing the present invention, reference is made to the drawings, wherein there
is seen a preferred embodiment shown schematically in Fig. 1. The drawing and the process it
represents will be described briefly below, without undue recitation of sensors, pumps,
indicators, transmitters, valves, pumps, and the like which are so well known to those skilled in
engineering systems of this type. Various labels are used in the drawings to have the meanings as
follows: TE = temperature element/sensor, LT = level transmitter/sensor, VFD = variable
frequency drive, SC = speed control, PI = pressure indicator/sensor, Tl = temperature
indicator/sensor, FT = flow transmitter, l/P - current to pressure transducer, FIT = flow indicating
transmitter, M = flowmeter, PLC = programmable logic controller.
[017] With reference to Fig. 1, a feed line 12 leads to urea tank 14 to maintain a sufficient
supply of an aqueous solution of urea or like chemical as described in United States Patent No.
7,090,810, the disclosure of which is incorporated herein by reference. The process is effective
with urea, but can utilize other NOx-reducing reagents capable of generating a reactant gas
containing ammonia upon heating. As will be clear from the following, when certain of these
reagents are gasified, the reactant gas will also contain HNCO which reacts with water to convert
to ammonia and carbon dioxide. It is an advantage of the invention that this can be easily
achieved without prehydrolysis of the NOx-reducing reagent which has the attendant risk of
plugging nozzles and other equipment. By the term "gasification" we mean that substantially all
of the urea is converted into a gas, leaving no significant dissolved or free solids or liquid to
contact with and foul SCR catalysts.
[018] The term "urea" is meant to include the reagents that are equivalent to urea in the
sense that they form ammonia and HNCO when heated, whether or not they contain large
amounts of the pure chemical urea in the form introduced into the combustion gases; however,
the reagents that are equivalent to urea typically contain measurable quantities of urea in their
commercial forms and thus comprise urea. Among the NOx-reducing reagents that can be
gasified are those that comprise a member selected from the group consisting of: ammelide;
ammeline; ammonium carbonate; ammonium bicarbonate; ammonium carbamate; ammonium
cyanate; ammonium salts of inorganic acids, including sulfuric acid and phosphoric acid;
ammonium salts of organic acids, including formic and acetic acid; biuret; triuret, cyanuric acid;
isocyanicacid; urea formaldehyde; melamine; tricyanourea and mixtures of any number of these.
Yet other NCvreducing reagents are available that do not form HNCO, but decompose to a
mixture of gases including hydrocarbons. Among this group are various amines and their salts
(especially their carbonates), including guanidine, guanidine carbonate, methyl amine carbonate,
ethyl amine carbonate, dimethyl amine carbonate, hexamethylamine; hexamethylamine
carbonate; and byproduct wastes containing urea from a chemical process. Amines with higher
alkyls can be employed to the extent that the hydrocarbon components released do not interfere
with the NOx-reduction reaction. The term "urea" is thus meant to encompass urea in all of its
commercial and equivalent forms. Typically, commercial forms of urea will consist essentially of
urea, containing 95% or more urea by weight. This relatively pure form of urea is preferred and
has several advantages in the process of the invention. It is preferably supplied to tank 14 at a
concentration of from about 10 to about 50%, with about 30 to about 35%.
[019] A level sensor and feed pump arrangement assure that sufficient urea solution will
always be present in the tank 14 to meet programmed demand. From the tank 14, which can be
heated to facilitate low temperature operation, the urea solution flows via line 16 assisted by
metering pump 18 and flow monitor 20 to line 22 for introduction through injector nozzle 24,
which with the aid of air from line 26, atomizes the aqueous urea solution for its gasification in
gasification chamber 28. The gasification of the urea is facilitated with heated air from line 34
which passes it to heater 36 and line 38 and auxiliary heater 39 for supply to chamber 28. In
chamber 28, the aqueous urea solution is heated at conditions of temperature (e.g., from about
175° to about 650°C) and pressure (e.g., at near atmospheric, say from about 0.5 to about 1.5
atm) for a time effective to gasify the urea and water by mixing the aqueous urea with the
heated gas stream from line 38 in amounts relative to the amounts of urea and water to produce
a first gasified reductant stream comprising a predetermined concentration of ammonia. A
typical gas stream will contain from about 0.5% to about 5% by weight ammonia. In some
embodiments, an air line 30 can be employed to aspirate the nozzle 24 during cleaning. The
gasified urea solution, also called gasified reductant, is withdrawn from chamber 28 via line 40
for distribution as a first gasified reductant stream to supply lines 42 serving the SCR units
associated with each of the turbines as will be describe more below.
[020] The demand for urea is monitored by sensors at each of the plurality of turbines by
sensing at least one control parameter of the combustion gases from a turbine which is indicative
of the NOx in the combustion gases and determining the demand by control programmable logic
controller 43 or other like device. The controller can be feed forward with or without feedback.
The first gasified reductant stream is fed to each turbine via individual lines 42, utilizing control
valves and flow monitors shown generally as 44 and 44', respectively, at a rate sufficient to
supply gasified reductant to supply the monitored demand to the selective catalytic NOx
reduction catalyst associated with each turbine. Because the turbines will have different
requirements for NOx reduction due to their loads, fuels supplied or other factors, and because
the gasified reductant must be uniformly dispersed within the combustion gases, normal
ammonia injection grids, AIGs, will not provide the desired distribution with effective reagent
utilization.
[021] Fig. 2 is a schematic representation of a single turbine with an SCR unit supplied with
gasified reductant in accord with the invention. The turbine 70 is fed fuel from line 72 and air
from line 74 and generates combustion gases 76 which pass into SCR unit 78 where they are
treated according to the invention and then exhausted to stack 80.
[022] Fig. 3 shows one form of AIG, ammonia injection grid 62, the operation of which in an SCR
system that can be improved according to the invention. Such grids will generally have an array
of pipes 63 with an array of holes 64 through which the gasified reagent is distributed to the
combustion gases from the associated turbine. The SCR unit includes an AIG, ammonia injection
grid, 62 fed gasified reagent via line 60.
[023] An in-line mixing device 65 is typically provided for assuring good mixing of the gasified
reagent with the combustion gases. Then, the gases are passed through a series of catalysts
effective for selective catalytic reduction of NOx at the designed temperatures of the system at
this point.
[024] Referring again to Fig. 1, it can be seen that the gasified reagent is passed via line 40 to
individual lines 42 to be mixed with a sufficient amount of carrier gas so that the correct dosing
of gasified reagents can be utilized and mixed with sufficient carrier gas to achieve the correct
mass flow rate and velocity profile for the reducing gas when introduced into the SCR unit 78 by
means of an injection grid 62.
[025] A separate supply system is provided for providing carrier gas to each individual turbine.
Fig. 1 shows air introduced via line 45 and blower 46 to heater 48 and line 50. The rates of supply
and degrees of heating can be controlled by appropriate sensors via controller 43 using
instrument air 43' or equivalent. Because the load of one or more turbines may not be high
enough to require sufficient ammonia that the flow through a feed line 42 maintains it at the
proper temperature, it is important that heater 48 be employed to maintain the temperature of
the gasified reagent in line 60.
[026] To achieve the advantages of the invention, the controller 43 or other logic device will
determie the amount of carrier gas needed to achieve a predetermined degree of mixing of the
gasified reagent with combustion gases generated at each turbine. Then, based on this
determination, a determined amount of carrier gas from supply line 50 and individual lines 52 is
admixed with the first gasified reductant stream from lines 40, 42 to provide a catalyst feed
stream associated with each turbine and which can be fed to the turbine via a line 60. Then, at
each turbine 70, an associated catalyst feed stream 60 is introduced by means of an ammonia
injection grid 62 to the combustion gases upstream of the catalyst 66 under conditions effective
to reduce the concentration of NOx in the effluent from each turbine. Similarly as with supply of
the first gasified reductant stream via individual lines 42, lines 52 can utilize control valves and
flow monitors shown generally as 54 and 54', respectively to control the rate sufficient to supply
a catalyst feed stream with the necessary mass and flow rate to each turbine.
[027] It is an advantage of the invention that a gasified product of urea can be fed with the
ability to fully control separate SCR units without excessive reagent usage or loss of pollution
control effectiveness. The controller 43 can determine the amount of reagent required for each
turbine to control NOx emissions and then direct mixing the gasified urea with the correct
amount of carrier gas for efficient operation of each separate SCR unit despite the demand
variation between the turbines. In this manner the gasification unit can be properly controlled to
provide urea on demand without the need for storing large inventories of ammonia-containing
gasses to correct for fluctuations in demand. While the description exemplifies turbines due to
the special effectiveness and importance of the invention in that context, it will be apparent to
those skilled in the art that its advantages can be extended to other types of combustors,
including furnaces, boilers, engines, incinerators and the like. It is another advantage of the
invention that the temperature of the gasified reagent in line 60 can be maintained at a
sufficient temperature to prevent condensation or chemical reactions even when the load of one
or more turbines may not be high enough for sufficient mass flow through a feed line 42.
[028] The above description is for the purpose of teaching the person of ordinary skill in the
art how to practice the invention. It is not intended to detail all of those obvious modifications
and variations, which will become apparent to the skilled worker upon reading the description. It
is intended, however, that all such obvious modifications and variations be included within the
scope of the invention which is defined by the following claims. The claims are meant to cover
the claimed components and steps in any sequence which is effective to meet the objectives
there intended, unless the context specifically indicates the contrary.
What is Claimed is:
1. A process for reducing the concentration of nitrogen oxides in combustion gases from a
plurality of turbines, each of which has an associated selective catalytic NOx reduction catalyst
effective for utilizing gasified urea, the process comprising:
a. heating aqueous urea at conditions of temperature and pressure for a time
effective to gasify the urea and water by mixing the aqueous urea with a heated
gas stream in amounts relative to the amounts of urea and water to produce a
first gasified reductant stream comprising a predetermined mass and
concentration of ammonia;
b. monitoring the demand for urea at each of the plurality of turbines;
c. feeding the first gasified reductant stream to each turbine at a rate sufficient to
supply gasified reductant to supply the monitored demand to the selective
catalytic NOx reduction catalyst associated with each turbine;
d. determining an amount of carrier gas needed to achieve a predetermined degree
of mixing of the gasified reagent with combustion gases generated at each
turbine;
e. based on this determination, admixing a determined amount of carrier gas with
the first gasified reductant stream to provide a catalyst feed stream associated
with each turbine; and
f. at each turbine, introducing an associated catalyst feed stream by means of an
ammonia injection grid to the effluent upstream of the catalyst under conditions
effective to reduce the concentration of NOx in the combustion gases from each
turbine.
2. A process for reducing the concentration of nitrogen oxides in combustion gases from a
plurality of combustors, each of which has an associated selective catalytic NOx reduction
catalyst effective for utilizing gasified urea, the process comprising:
a. heating aqueous urea at conditions of temperature and pressure for a time
effective to gasify the urea and water by mixing the aqueous urea with a heated
gas stream in amounts relative to the amounts of urea and water to produce a
first gasified reductant stream comprising a predetermined mass and
concentration of ammonia;
b. monitoring the demand for urea at each of the plurality of combustors;
c. feeding the first gasified reductant stream to each combustor at a rate sufficient
to supply gasified reductant to supply the monitored demand to the selective
catalytic NOx reduction catalyst associated with each combustor;
d. determining an amount of carrier gas needed to achieve a predetermined degree
. of mixing of the gasified reagent with combustion gases generated at each
combustor;
e. based on this determination, admixing a determined amount of carrier gas with
the first gasified reductant stream to provide a catalyst feed stream associated
with each combustor; and
f. at each combustor, introducing an associated catalyst feed stream by means of an
ammonia injection grid to the effluent upstream of the catalyst under conditions
effective to reduce the concentration of NOx in the combustion gases from each
combustor.



Disclosed is a system which enables the efficient utilization of urea for selective catalytic reduction (SCR) of NOx
by gasifying it and feeding it to a plurality of selective catalytic reduction units associated with a plurality of gas turbines. The
invention enables feeding a gasified product of the urea with the ability to fully control separate SCR units without excessive reagent
usage or loss of pollution control effectiveness. Controllers determine the amount of reagent required for each turbine to control
NOx emissions and then mixes the gasified urea with the correct amount of carrier gas for efficient operation of each separate SCR
unit despite the demand variation between the turbines. In this manner the gasification unit can be properly controlled to provide
urea on demand without the need for storing large inventories of ammonia-containing gasses to correct for fluctuations in demand.

Documents:

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Patent Number 268585
Indian Patent Application Number 1735/KOLNP/2010
PG Journal Number 37/2015
Publication Date 11-Sep-2015
Grant Date 04-Sep-2015
Date of Filing 13-May-2010
Name of Patentee FUEL TECH, INC
Applicant Address 27601 BELLA VISTA PARKWAY, WARRENVILLE, IL 60555 U.S.A
Inventors:
# Inventor's Name Inventor's Address
1 BOYLE, JOHN, M. 1047 N. LOMBARD AVENUE, OAK PARK, IL 60302 U.S.A
2 SUN, WILLIAM, H. 2285 PEBBLE CREEK DRIVE, LISLE, IL 60532 U.S.A
3 CARMIGNANI, PAUL, G. 908 BROCKS END COURT, NAPERVILLE, IL 60540 U.S.A
PCT International Classification Number B01D 53/86
PCT International Application Number PCT/US2008/082925
PCT International Filing date 2008-11-09
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 60/986,917 2007-11-09 U.S.A.