HIT LOGO

HALDIA INSTITUTE OF TECHNOLOGY

2014
SELECTIVE CATALYTIC
REDUCTION OF NOX
Submitted By:
Kushagra Abhishek
11/CH/25
H A L D I A I N S T I T U T E O F T E C H N O L O G Y
SELECTIVE CATALYTIC REDUCTION OF NOX

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CONTENTS
Page no.
Preface 3
Acknowledgement 4
Abstract 5
Introduction 6
What is NOX 6
Contribution of NOx to atmosphere by
various sources
6
Why should be control NOx 7
Types of NOX formation 10
What is selective catalytic reduction of
NOX
14
How does ammonia reduce Nitrogen
Oxide?
14
SCR catalysts 18
How catalysts works in SCR technology 18
Limitation of SCR of NOx 19
CONCLUSION 20
References 21




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Preface
Presence of nox in air us very harmful and dangerous to all of living organism of
biosphere.
These toxic gases are emitted by human activity like automobiles, industry boilers,
furnace kiln operation and many other.
Exhaust coming out of these is very toxic so they are treated before releasing it into
environment.
There are various methods involves in treatment of this flue gas
In this report one of the most efficient method have been put in detail. This method
is very simple, clean and reliable method with highest efficiency. This is nothing
but SELECTIVE CATALYTIC REDUCTION OF NOx .


















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Acknowledgement
I would like to thank Mr. Biswajeet Mondal sir , Astt. Prof. at HIT Haldia for
giving me a very challenging and interesting project on selective catalytic
reduction of NOx . His proper guidance and instruction throughout the project
work keeps me energetic and enthusiastic. I would like to thank him again for
giving me a wonderful opportunity to have a firsthand report and presentation
experience. I would also like to thank Dr. R.N. Jana sir and DR. Avijit Ghosh sir
(both Astt. Prof). for their valuable assistance throughout the project As and when
required.
At last but not the least I would also like to thank my friends on presentation and
report preparation related issues.

















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Abstract

The SCR technology for reducing nitrogen oxides (NOx) finds applications
worldwide as an after treatment system for power plants and waste furnaces.
Ammonia (NH3) could also be used directly as a reagent, but the solution of urea
in water is by far the best reagent since it is a non-toxic product and there are no
restrictions for its transport on rail, road or ships. Furthermore, urea is a product
largely used in agriculture and in industry and urea of various quality grades is
readily available. An oxidation catalyst may be used to improve the efficiency of
the SCR by converting NO into NO2 and by oxidising CO and hydrocarbons.
Accurate dosing of the urea solution and appropriate strategies during transient
modes prevent an NH3 slip. The SCR technology, by converting directly NOx to
N2 outside the engine, allows the retaining of the engine calibrations, which
correspond to the best compromise between fuel consumption and the formation of
pollutants during the combustion process














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INTRODUCTION

What is NOX?
Nitrogen oxides (NOx) are a very interesting and important family of air polluting
chemical Compounds. NO
x
is a generic term for mono-nitrogen oxides NO and
NO
2
(nitric oxide and nitrogen dioxide). They are produced from the reaction
of nitrogen and oxygen gases in the air during combustion, especially at high
temperatures. In areas of high motor vehicle traffic, such as in large cities, the
amount of nitrogen oxides emitted into the atmosphere as air pollution can be
significant. NO
x
gases are formed whenever combustion occurs in the presence of
nitrogen as in an air-breathing engine; they also are produced naturally
by lightning. In atmospheric chemistry, the term means the total concentration of
NO and NO
2
. NO
x
gases react to form smog and acid rain as well as being central
to the formation of tropospheric ozone.


Contribution of NOx to atmosphere by various sources is depicted below in fig:1



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Fig:1

WHY SHOULD WE CONTROL NOx?
NOx represent a family of seven compounds. Actually, EPA(Environmental
Protection Agency) regulates only nitrogen dioxide (NO2) as a surrogate for this
family of compounds because it is the most prevalent form of NOx in the
atmosphere that is generated by anthropogenic (human) activities. NO2 is not only
an important air pollutant by itself, but also reacts in the atmosphere to form ozone
(O3) and acid rain. It is important to note that the ozone that we want to minimize
is tropospheric ozone; that is, ozone in the ambient air that we breathe.Actually
Stratospheric ozone protects us and the troposphere from ionizing radiation coming
from the sun. EPA has established National Ambient Air Quality Standards
(NAAQS) for NO2 and Tropospheric ozone. The NAAQS define levels of air
quality that are necessary, with a Reasonable margin of safety, to protect public
health (primary standard) and public welfare (Secondary standard) from any
known or anticipated adverse effects of pollution. The primary and secondary
standard for NO2 is 0.053 parts per million (ppm) (100 micrograms per cubic
meter), annual arithmetic mean concentration.



Fig:2

The NO in air, then reacts with free radicals in the atmosphere, which are
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also created by the UV acting on volatile organic compounds (VOC). The free
radicals then recycle NO to NO2. In this way, each molecule of NO can produce
ozone multiple times.40 This will continue until the VOC are reduced to short



chains of carbon compounds that cease to be photo reactive (a reaction caused by
light). A VOC molecule can usually do this about 5 times.
In addition to the NO2 and Ozone NAAQS concerns, NOx and sulfur oxides (SOx)
in the atmosphere are captured by moisture to form acid rain. Acid rain, along with
cloud and dry deposition, severely affects certain ecosystems and directly affects
some segments of our economy. All of these facts indicate an obvious need to
reduce NOx emissions. However, to successfully do so, we must understand the
generation and control of the NOx family of air pollutants. picture depicted in fig:1
is indicating the overall situation as mentioned preceding lines.








WHAT IS A NITROGEN OXIDE?

Diatomic molecular nitrogen (N2) is a relatively inert gas that makes up about
80% of the air we breathe. However, the chemical element nitrogen (N), as a single
atom, can be reactive and have ionization levels (referred to as valence states) from
plus one to plus five. Thus nitrogen can form several different oxides. Using the
Niels Bohr model of the atom, valence state relates to the number of electrons
which are either deficient (positive valence) or surplus (negative valence) in the
ion when compared with the neutral molecule. The family of NOx compounds
and their properties are listed in Table 1.

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Oxygen ions are always at valence minus 2. Depending upon the number of oxygen ions (always
balanced by the valence state of nitrogen), NOx can react to either deplete or enhance ozone
concentrations. The nitrogen ion in these oxides really does a dance in which it has (at different
times) various numbers of oxygen ions as partners. Nitrogen changes its number of partners
when it changes its ionization energy level. This happens whenever NOx:

(1) is hit with a photon of ionizing radiation (UV or a shorter wavelength light)
(2) is hit with enough photons that together transfer enough energy to change its ionization level
(3) is catalyzed
(4) is stimulated sufficiently by thermal (IR) energy
(5) reacts with a chemically oxidizing or reducing radical (an ionized fragment of a molecule);
(6) reacts with a chemically oxidizing or reducing ion (an atom with unbalanced electrical
charge).
When any of these oxides dissolve in water and decompose, they form nitric acid (HNO3) or
nitrous acid (HNO2). Nitric acid forms nitrate salts when it is neutralized. Nitrous acid forms
nitrite salts. Thus, NOx and its derivatives exist and react either as gases in the air, as acids in
droplets of water, or as a salt. These gases, acid gases and salts together contribute to pollution
effects that have been observed and attributed to acid rain.
Nitrous oxide (N2O), NO, and NO2 are the most abundant nitrogen oxides in the air. N2O (also
known as laughing gas) is produced abundantly by biogenic sources such as plants and yeasts. It
is only mildly reactive, and is an analgesic
N2O is an ozone depleting substance which reacts with o
3
in both the troposphere and
stratosphere.
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Except for NO from soils, lightning and natural fires, NO is largely anthropogenic (i.e.,
generated by human activity). Biogenic sources are generally thought to account for less than
10% of total NO emissions.



WHERE DOES NOx COME FROM?
Automobiles and other mobile sources contribute about half of the NOx that is emitted. Electric
power plant boilers produce about 40% of the NOx emissions from stationary sources.
Additionally, substantial emissions are also added by such anthropogenic sources as industrial
boilers, incinerators, gas turbines, reciprocating spark ignition and Diesel engines in stationary
sources, iron and steel mills, cement manufacture, glass manufacture, petroleum refineries, and
nitric acid manufacture. Biogenic or natural sources of nitrogen oxides include lightning, forest
fires, grass fires, trees, bushes, grasses, and yeasts.1 These various sources produce differing
amounts of each oxide. The anthropogenic sources are approximately shown as:




This shows a graphic portrayal of the emissions of our two greatest sources of NOx. If we
could reduce the NOx emissions from just these two leading categories, we might be able to live
with the rest. However, dont expect either of these categories to become zero in the foreseeable
future. We cannot expect the car, truck, bus, and airplane to disappear. The zero-emission car is
still on the drawing board and not on the production line. Also, social customs will have to
change before consumption of electricity can be reduced.


In all combustion there are three opportunities for Types of NOx formation. They are:
1. Thermal NOx - The concentration of thermal NOx is controlled by the nitrogen and
oxygen molar concentrations and the temperature of combustion. Combustion at temperatures
well below 1,300_C (2,370_F) forms much smaller concentrations of thermal NOx.
2. Fuel NOx - Fuels that contain nitrogen (e.g., coal) create fuel NOx that results from
oxidation of the already-ionized nitrogen contained in the fuel.
3. Prompt NOx - Prompt NOx is formed from molecular nitrogen in the air combining with fuel
in fuel-rich conditions which exist, to some extent, in all combustion. This nitrogen then oxidizes
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along with the fuel and becomes NOx during combustion, just like fuel NOx. The abundance of
prompt NOx is disputed by the various writers of articles and reports - probably because they
each are either considering fuels intrinsically containing very large or very small amounts of
nitrogen, or are considering burners that are intended to either have or not have fuel-rich regions
in the flame.

Table 2 lists principles or methods that are used to reduce NOx. Basically there are six:





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Method 1. Reducing Temperature -- Reducing combustion temperature means avoiding the
stoichiometric ratio (the exact ratio of chemicals that enter into reaction). Essentially, this
technique dilutes calories with an excess of fuel, air, flue gas, or steam. Combustion controls use
different forms of this technique and are different for fuels with high and low nitrogen content.

Control of NOx from combustion of high nitrogen content fuels (e.g., coal) can be understood by
the net stoichiometric ratio. Control of the NOx from combustion of low nitrogen fuels (such as
gas and oil) can be seen as lean versus rich fuel/air ratios. Either way, this technique avoids the
ideal stoichiometric ratio because this is the ratio that produces higher temperatures that generate
higher concentrations of thermal NOx.
Combustion temperature may be reduced by: (1) using fuel rich mixtures to limit the amount of
oxygen available; (2) using fuel lean mixtures to limit temperature by diluting energy input;
(3) injecting cooled oxygen-depleted flue gas into the combustion air to dilute energy;
(4) injecting cooled flue gas with added fuel; or (5) injecting water or steam. Low-NOx burners
are based partially on this principle.8,9,10 The basic technique is to reduce the temperature of
combustion products with an excess of fuel, air, flue gas, or steam. This method keeps the vast
majority of nitrogen from becoming ionized (i.e., getting a non-zero valence).


Method 2. Reducing Residence Time -- Reducing residence time at high combustion
temperatures can be done by ignition or injection timing with internal combustion engines. It can
also be done in boilers by restricting the flame to a short region in which the combustion air
becomes flue gas. This is immediately followed by injection of fuel, steam, more combustion
air, or recirculating flue gas. This short residence time at peak temperature keeps the vast
majority of nitrogen from becoming ionized. This bears no relationship to total residence time
of a flue gas in a boiler.


Method 3. Chemical Reduction of NOx This technique provides a chemically reducing (i.e.,
reversal of oxidization) substance to remove oxygen from nitrogen oxides. Examples include
Selective Catalytic Reduction (SCR) which uses ammonia, Selective Non-Catalytic Reduction
(SNCR) which use ammonia or urea, and Fuel Reburning (FR). Non-thermal plasma, an
emerging technology, when used with a reducing agent, chemically reduces NOx. All of these
technologies attempt to chemically reduce the valence level of nitrogen to zero after the valence
has become higher.11 Some low-NOx burners also are based partially on this principle.


Method 4. Oxidation of NOx -- This technique intentionally raises the valence of the nitrogen
ion to allow water to absorb it (i.e., it is based on the greater solubility of NOx at higher
valence).
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This is accomplished either by using a catalyst, injecting hydrogen peroxide, creating ozone
within the air flow, or injecting ozone into the air flow. Non-thermal plasma, when used without
a reducing agent, can be used to oxidize NOx. A scrubber must be added to the process to
absorb N2O5 emissions to the atmosphere. Any resultant nitric acid can be either neutralized by
the scrubber liquid and then sold (usually as a calcium or ammonia salt), or collected as nitric
acid to sell to customers.12, 49



Method 5. Removal of nitrogen from combustion -- This is accomplished by removing
nitrogen as a reactant either by: (1) using oxygen instead of air in the combustion process; or
(2) using ultra-low nitrogen content fuel to form less fuel NOx. Eliminating nitrogen by using
oxygen tends to produce a rather intense flame that must be subsequently and suitably diluted.
Although Method 2 can lower the temperature quickly to avoid forming excessive NOx, it
cannot eliminate nitrogen oxides totally if air is the quench medium. Hot flue gas heats the air
that is used to quench it and this heating generates some thermal NOx. This method also includes
reducing the net excess air used in the combustion process because air is 80% nitrogen. Using
ultra-low-nitrogen content fuels with oxygen can nearly eliminate fuel and prompt NOx.13

Method 6. Sorption, both adsorption and absorption -- Treatment of flue gas by injection of
sorbents (such as ammonia, powdered limestone, aluminum oxide, or carbon) can remove NOx
and other pollutants (principally sulfur). There have been successful efforts to make sorption
products a marketable commodity. This kind of treatment has been applied in the combustion
chamber, flue, and baghouse. The use of carbon as an adsorbent has not led to a marketable
product, but it is sometimes used to limit NOx emissions in spite of this. The sorption method is
often referred to as using a dry sorbent, but slurries also have been used. This method uses either
adsorption or absorption followed by filtration and/or electrostatic precipitation to remove the
sorbent.


Method 7. Combinations of these methods -- Many of these methods can be combined to
achieve a lower NOx concentration than can be achieved alone by any one method. For example,
a fuel-rich cyclone burner (Method 1) can be followed by fuel reburn (Method 3) and over-fire
air (Method 1). This has produced as much as a 70% reduction in NOx.55 Other control
technologies that are intended to primarily reduce concentrations of sulfur also strongly affect
the nitrogen oxide concentration. For example, the SOx-NOx-ROx-Box (SNRB) technology uses
a limestone sorbent in the flue gas from the boiler to absorb sulfur. This is followed by ammonia
injection and SCR using catalyst fibers in the baghouse filter bags. The sulfur is recovered from
the sorbent and the sorbent regenerated by a Claus process. This has demonstrated removal of up
to 90% of the NOx along with 80% of the SOx.39, 42 EBARA of Japan reported that an electron
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beam reactor with added ammonia removed 80% of the SO2 and 60% of the NOx for a utility
boiler in China.54 FLS Milo and Sons reported at the same symposium that 95% of the SO2 and
70%-90% of the NOx were removed in several demonstrations of their SNAP technology, which
is based upon an aluminum oxide adsorber with Claus regeneration.


Selective catalytic reduction technology for reducing content of NOx in air/flue gas.
Q.)What is scr?
Ans.) SCR uses a catalyst to react injected ammonia to chemically reduce NOx. It
can achieve up to a 94% reduction in NOx and is one of the most effective NOx
abatement techniques. However, this technology has a high initial cost. In addition,
catalysts have a finite life in flue gas and some ammonia slips through without
being reacted. SCR has historically used precious metal catalysts, but can now also
use base-metal and zeolite catalysts. The base-metal and operate at much different
temperatures then the precious metal catalysts

Selective catalytic reduction (SCR) -Involves using beds containing ammonia or
urea to reduce nitrogen oxides to molecular nitrogen and water. Two or three
catalysts (usually tungsten and vanadium) are arranged in honeycomb shapes in
the beds so air can flow through. NOx reduction efficiencies ranging from 75 to
90% are possible when the amount of catalyst is sufficient, the catalyst is in good
condition, the ammonia reagent flow is sufficient, and the ammonia is adequately
distributed across the gas stream.
How does ammonia reduce Nitrogen Oxide?
Injection of ammonia in the flue gas in presence of a catalyst which causes
chemical reactions that convert the NOx to free nitrogen and water vapor.

NO
4 NO + 4 NH3 + O2 ----------- 4 N2 + 6 H2O

NO2
4 NO2 + 8 NH3 + 2 O2 ----------- 6 N2 + 12 H2O
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Temperatures for ideal de-nitrification must take place between 392 and 1022
degree Fahrenheit. Temperatures below 400 can cause the formation of ammonia
salts. Temperatures above 850 can cause a reverse reaction where ammonia is
converted back into NOx. There are various operation modes of a combined cycle
power plant, which inherently require varying amounts of ammonia to be injected
into the flue gas stream as part of the SCR system. In SCR systems, ammonia or a
compound of ammonia is used as the reducing agent and is injected into the flue
gas stream, passing over a catalyst. NOx emission reductions over 80-90% are
achieved. Temperatures for ideal de-nitrification must take place between 392F
and 1022F. Temperatures below 400F can cause the formation of ammonia salts.
Temperatures above 850F can cause a reverse reaction where ammonia
is converted back into NOx.
several secondary reactions during reduction of NOx by NH3 are:
2SO
2
+ O
2
2SO
3

2NH
3
+ SO
3
+ H
2
O (NH4)2SO4
NH
3
+ SO
3
+ H
2
O NH
4
HSO
4


Note: The reaction for urea instead of either anhydrous or
aqueous ammonia is:
4NO + 2(NH
2
)
2
CO + O
2
4N
2
+ 4H
2
O + 2CO
2


SCR CATALYSTS:
SCR catalysts are manufactured from various ceramic materials used as a
carrier, such as titanium oxide, and active catalytic components are usually
either oxides of base metals (such vanadium, molybdenum and tungsten),
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zeolites, or various precious metals. Each catalyst component has
advantages and disadvantages.
Base metal catalysts, such as the vanadium and tungsten, lack high
thermal durability, but are less expensive and operate very well at the
temperature ranges most commonly seen in industrial and utility boiler
applications. Thermal durability is particularly important for automotive SCR
applications that incorporate the use of a diesel particulate filter with forced
regeneration. They also have a high catalyzing potential to oxidize SO
2 into SO3, which can be extremely damaging due to its acidic properties.
Zeolite catalysts have the potential to operate at substantially higher
temperature than base metal catalysts; they can withstand prolonged
operation at temperatures of 900 K and transient conditions of up to
1120 K. Zeolites also have a lower potential for potentially damaging SO
2 oxidation.Iron- and copper-exchanged zeolite urea SCRs have been
developed with approximately equal performance to that of vanadium-urea
SCRs if the fraction of the NO2 is 20% to 50% of the total NOx. The two
most common designs of SCR catalyst geometry used today
are honeycomb and plate. The honeycomb form usually is
an extruded ceramic applied homogeneously throughout the ceramic
carrier or coated on the substrate. Like the various types of catalysts, their
configuration also has advantages and disadvantages. Plate-type catalysts
have lower pressure drops and are less susceptible to plugging and fouling
than the honeycomb types, but plate configurations are much larger and
more expensive. Honeycomb configurations are smaller than plate types,
but have higher pressure drops and plug much more easily. A third type is
corrugated, comprising only about 10% of the market in power plant
applications.

Reductants:
Several reductants are currently used in SCR applications
including anhydrous ammonia, aqueous ammonia or urea. All those three
reductants are widely available in large quantities.
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Pure anhydrous ammonia is extremely toxic and difficult to safely store, but
needs no further conversion to operate within an SCR. It is typically
favoured by large industrial SCR operators. Aqueous ammonia must
be hydrolyzed in order to be used, but it is substantially safer to store and
transport than anhydrous ammonia. Urea is the safest to store, but requires
conversion to ammonia through thermal decomposition in order to be used
as an effective reductant.


SCR technology working stepsin boiler is shown below in Fig:3


Fig:3
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How catalysts works in SCR technology
In SCR method there is a bed of catalyst arranged in Plate configuration or Honey
comb configuration.
There are two beds of catalyst for ex: in V &Ti or Pt/Pd or Rh type catalyst
arrangement, when flue gas coming from exhaust of silencer of automobiles then
there is ammonia injection in the path of flue gas. As we know flue gas are
composed of harmful nox gases then reduction reaction takes place. Here
catalyst bed attracts or bind towards itself N2 . Again at second bed of catalysts
hydrocarbon oxidise co. This co reacts with O2 to get less harmful Co2 gas and
water vapour. At last there is a control system to regulate and keep air fuel ratio
at optimum level. This situation is depicted as shown below in Fig:4



Fig:4

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Limitation of SCR of NOx:
SCR systems are sensitive to contamination and plugging resulting from
normal operation or abnormal events. Many SCRs are given a finite life due
to known amounts of contaminants in the untreated gas. The large majority
of catalyst on the market is of porous construction. A clay planting pot is a
good example of what SCR catalyst feels like. This porosity is what gives
the catalyst the high surface area essential for reduction of NOx. However,
the pores are easily plugged by a variety of compounds present in
combustion/flue gas. Some examples of plugging contaminates are: fine
particulate, ammonia sulfur compounds, ammonium bisulfate (ABS) and
silicon compounds. Many of these contaminants can be removed while the
unit is on line, for example by soot blowers. The unit can also be cleaned
during a turnaround or by raising the exhaust temperature. Of more
concern to SCR performance is poisons, which will destroy the chemistry of
the catalyst and render the SCR ineffective at NOx reduction or cause
unwanted oxidation of ammonia (forming more NOx). Some of these
poisons include: halogens, alkaline metals, arsenic, phosphorus, antimony,
copper.
Most SCRs require tuning to properly perform. Part of tuning involves
ensuring a proper distribution of ammonia in the gas stream and uniform
gas velocity through the catalyst. Without tuning, SCRs can exhibit
inefficient NOx reduction along with excessive ammonia slip due to not
utilizing the catalyst surface area effectively. Another facet of tuning
involves determining the proper ammonia flow for all process conditions.
Ammonia flow is in general controlled based on NOx measurements taken
from the gas stream or preexisting performance curves from an engine
manufacturer (in the case of gas turbines and reciprocating engines).
Typically, all future operating conditions must be known beforehand to
properly design and tune an SCR system.
Ammonia slip is an industry term for ammonia passing through the SCR
un-reacted. This occurs when ammonia is: over-injected into gas stream;
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temperatures are too low for ammonia to react; or catalyst has degraded
(see above).
Temperature is one of the largest limitations of SCR. Gas turbines, cars,
and diesel engines all have a period during a start-up where exhaust
temperatures are too cool for NOx reduction to occur.


CONCLUSION:
Selective catalytic reduction of NOx is very simple, clean and reliable
technique for reducing NOx content in flue gas.
Although its initial installation cost is high but its efficiency in reducing nox
is upto 95%,largest by any other available technology. This technique
enhances engine life of automobile, also less consumption of fuel.
Staging of the combustion is implicit in several pollution prevention
techniques. Tandem application (or use of hybrid control technology) of
NOx control techniques (first SNCR, then SCR in the duct, and then
sorption before the ESP which is referred to as polishing) have been used
to achieve an overall reduction of 90+% in NOx and 80% in SOx, even
without using low- NOx burners to lower NOx generation












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References:

1. Nitrogen Oxides (NOx),Why and How They Are
Controlled by Clean Air Technology Center (MD-12)
Information Transfer and Program Integration Division
Office of Air Quality Planning and Standards
U.S. Environmental Protection Agency

2. Selective Catalytic Reduction
(Final Report) by ACEA.

3. Effects of Nitrogen Oxides". Electric Power Research Institute, 1989

4) Gieshoff, J; M. Pfeifer, A. Schafer-Sindlinger, P. Spurk, G. Garr, T.
Leprince (March 2001). "Advanced Urea Scr Catalysts for Automotive
Applications" (PDF). Society of Automotive Engineers. Retrieved 2009-05-

4. "NOx Removal". Branch Environmental Corp. Archived from the original on 2007-10-
08. Retrieved 2007-12-26.

5. http://en.wikipedia.org/wiki/Selective_catalytic_reduction

6. www.epa.gov/ttncatc1/dir1/fnoxdoc.pdf