United States
 Environmental Protection
 Agency
 Industrial Environmental Research
 Laboratory
 Research Triangle Park NC 27711
 Research and Development
 EPA-600/S7-83-027 July 1983
 Project  Summary
 NOx Abatement  for Stationary
 Sources  in Japan
Jumpei Ando
  Strict ambient air quality standards
for SQ2 and NO,, in Japan mandate the
use of various air pollution technologies.
This report is a compilation of informa-
tion on the current status of NOX abate-
ment technologies for stationary sources
in Japan.  The author obtained this
information from electric power com-
panies, various industries,  and de-
velopers of numerous technology pro-
cesses as well as from his own original
research in the field. The report focuses
on the Combustion Modification (CM)
and Selective Catalytic Reduction (SCR)
NO, abatement technologies. Informa-
tion is provided on the development
status, pilot and demonstration  plant
tests, technological problems,  and
costs associated with the use of these
technologies in Japan. Detailed opera-
tion  data  are given  to describe the
commercial operation of SCR plants.
  This Project Summary was developed
by EPA's Industrial Environmental Re-
search Laboratory. Research Triangle
Park. NC, to announce key findings of
the research project that is fully doc-
umented in a separate report of the
same title (see Project Report ordering
information at back).
     Standards and Ambient
Concentrations
  Recent air pollution control efforts in
Japan have concentrated on NOX abate-
ment since ambient S02 concentrations
already have been drastically reduced in
response to stringent standards. In 1 978,
the ambient air quality standard for N02
was amended from 0.02 ppm to 0.04 -
0.06 ppm as a daily average.  In regions
with N02 concentrations above 0.06 ppm,
the concentration will be reduced to 0.06
ppm  by 1985.  In regions with N02
concentrations of 0.04 - 0.06 ppm, efforts
 will be made to keep the concentrations
 from substantially exceeding the present
 level  In areas with concentrations below
 0.04 ppm, efforts must be made to main-
 tain those levels. The new NO2 standard is
 relaxed compared with the previous stan-
 dard, 0.02 ppm as a daily average, but is
 still more stringent than the U.S. standard
 of 0.05 ppm as a yearly average.
  In regions  with large cities (such  as
Tokyo and Osaka), ambient N02 concen-
trations often exceed the standards, reach-
ing 0.07-0.08 ppm as daily averages. The
prefectoral governments of Chiba, Kanaga-
wa, and Mie have established even more
stringent regulations and plan to reduce
N02 concentrations to 0.04 ppm from the
current 0.05-0.06 ppm.  Even in regions
with N02 concentrations below 0.04 ppm,
NOX reduction is often required by local
governments  to prevent any  further in-
crease.
  Nearly 2 million tons/yr of NOX are
emitted in Japan, 60%  from stationary
sources and the rest from mobile sources.
In large cities such as Tokyo and Osaka,
about  60% of the NOX is emitted from
mobile sources.
  NOX  emissions from  gasoline-engine
passenger cars manufactured since 1978
have been controlled by stringent regula-
tions. The current limit is 0.25 g/km (8%
of the NOX emissions from cars in 1973).
NOX emissions from diesel-engine buses
and trucks have been reduced to about
50% of the 1974 level. For stationary
combustion sources, emission standards
based on advanced combustion modifica-
tion technology have been applied to re-
duce NOX by 30-70%.
  With these  efforts, ambient N02 con-
centrations are no longer increasing despite
a continuing increase in the number  of
stationary and mobile sources. However,
it is difficult to lower current N02 con-

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centrations in large cities and industrial
regions without more effective emission
controls for diesel-engine cars and sta-
tionary sources.


NOX Reduction for Stationary
Sources
  Nearly all NOX emissions are produced
by the combustion of  fossil  fuels.   In
Japan, the major combustion fuel is heavy
oil. This residue of the atmospheric distil-
lation of crude oil has been used at the rate
of nearly 200 million kl (kiloliters)/yr.  Coal
use decreased markedly between 1965
and 1 975 and currently accounts for only
3% of Japan's total energy supply.  How-
ever, coal consumption is  expected  to
triple in the next 10 years. Imported LNG
also accounts for about 3% of the energy
currently used and is expected to nearly
triple in 10 years.
  Large stationary sources such as utility
boilers have reduced NOX emissions 50-
7096 by applying  combustion modifica-
tions (CM) including low excess air com-
bustion, staged combustion, flue gas re-
circulation, and Iow-N0x burners.  As a
result the NOX concentration in  flue gas
from utility boilers  is minimal--150-300
ppm for coal, 80-120 ppm for oil, and 40-
60 ppm for gas firing. Smaller boilers and
furnaces  have reduced  NOX 30-50% by
using Iow-N0x burners or  by switching
from heavy oil to kerosene.
  For additional NOX abatement, several
flue gas treatment (FGT) processes have
been developed.   Of all the processes,
selective catalytic reduction (SCR), which
uses ammonia and a catalyst at 300-
400°C to control  NOX,  is presently the
most advanced  technology.  Over  1 50
commercial SCR plants are in operation to
remove 80-9096  of the NOX emissions.
Selective noncatalytic  reduction (SNR),
which uses ammonia at 800-1,000°C to
remove 30-5096 of IMOX emissions, has
been developed and applied to about 20
furnaces and industrial boilers. Wet and
dry simultaneous SOX and  NOX  removal
processes also have been developed but
have not been applied commercially except
for several small units.
  SCR has been used most often for flue
gas treatment because  of  its simplicity
(which enables unattended operation),
relatively high NOX removal efficiency (80-
9096), and relatively low cost Most of the
new coal-fired utility boilers being planned
will  have SCR units.  SCR will also be
needed for some of the existing boilers
even in regions with NOX concentrations
below a 0.04 ppm daily average, due to
local policies which forbid any increase in
NOX levels.  For example, when a  new
boiler is installed at a power station, not
only the new boiler, but also some of the
existing boilers, will be required to  have
SCR units so that total NOX emissions
from the station do not increase.
  SCR is usually used with CM.  For most
boilers and furnaces, CM  is applied  first
followed by  SCR in order to meet the
stringent regulations.  For over 90% NOX
reduction, the combination of CM (to re-
duce 35-50% of the NOX  emissions) and
SCR (to remove 80-8596 of the remaining
NOX) is usually more economical than SCR
by itself.
  Typical examples of  uncontrolled  and
controlled NOX concentrations  in utility
boiler flue gas are shown in  Table 1.
Examples of NOX regulations and emis-
sions from utility boilers are  shown in
Table 2.
  A new combustion process, in-furnace
NOX removal, has been developed to re-
move about  50% of NOX by injecting  a
small portion of the fuel above the flame,
followed by air addition to ensure complete
combustion.   Using this  process, along
with CM for utility boilers, NOX may be
reduced to 100 ppm for coal, 50 ppm for
oil,  and 20 ppm for gas.
  Fluidized-bed combustion, gasification,
and liquefaction of coal  all  have  been
tested in Japan, but these technologies
are not as advanced there as they are in the
U.S. This is  because Japan must import
coal and because these technologies are
unable to meet the stringent Japanese
NOX emission  regulations.  Most of the
                              new coal-fired boilers in Japan will use
                              conventional pulverized coal combustion
                              with CM, SCR, and FGD.

                              SCR and SCR/FGD
                              Characteristics
                                SCR problems of the past have been
                              solved by recent improvements. The major
                              problems were: 1) poisoning of the catalyst
                              by SOX in the gas, 2) dust plugging of the
                              catalyst, and 3) deposition of ammonium
                              bisulfate in the air preheater downstream
                              of the SCR reactor. Catalyst poisoning has
                              been eliminated by using catalysts based
                              on Ti02 instead of AI203 or Fe203- The
                              use of parallel-flow honeycomb, tube, or
                              plate catalysts or a parallel passage reactor
                              eliminates dust plugging.   Ammonium
                              deposits can be prevented by maintaining
                              the concentration of unreacted ammonia
                              in the reactor outlet gas below 5 ppm and
                              using  a low-oxidation catalyst To do this,
                              0.82 -0.95 mole NH3 is usually used per
                              mole NOX to obtain 80-90%  NOX removal
                              with less  than 5  ppm  unreacted NH3,
                              while  S02 oxidation is kept below 1 %.
                                SCR and FGD system applications to
                              boilers and other gas sources are shown
                              schematically in Figure 1.  SCR  is easily
                              applied to boiler economizer outlet gas al
                              300-400°C as shown in the A portion of
                              the figure. For S0x-rich gases, FGD may
                              be applied downstream of SCR as shown
                              in B.  At an  early  stage of development,
                              SCR was applied downstream  of FGD
                              systems, as  shown in  C, to protect the
                              catalyst from SOX attack System C, how-
                              ever, is expensive; it requires large amounts
Table 1.
Examples of Controlled and Uncontrolled NOX  Concentrations in Utility Boilei
Flue Gas
                    Outlet NOX Concentration, ppm
                                          Percent Control
Fuel
Gas
Oil
Coal
Without
Control,
ppm
200
300
600
Controlled
by
CM
50
WO
250
Controlled
by CM
and SCR
10
20
50
by CM
70
67
58
by SCR
83
80
80
Total
%
Control
95
93
91
Table 2.
Fuel
Gas
Gas
Oil
Oil
Coal
Coal
Examples of NOX Regulations and Emissions from Utility Boilers, ppm
Boiler Central Government Local Agreement Actual Emission
Existing
New
Existing
New
Existing
New
100
60
150
130
400
400
60
10
100
25
159C
170
60°
8"
WO3
20*
1703
160"
"By combustion modification (CM).
bBy CM and selective catalytic reduction (SCR).
cDesired by local government.
dBy CM and partial SCR

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of energy for gas reheating. System B has
become popular as S0x-resistant catalysts
have been developed.
  System D is often used for flue gas from
a low-sulfur coal. In this system, the boiler
economizer outlet gas is first treated by a
hot electrostatic precipitator (ESP)  and
then by SCR and FGD.  A cold ESP is not
highly efficient for flue gas from low-sulfur
coal. For high- and medium-sulfur coals,
system B is preferable. System B may also
be useful for low-sulfur coal if both the
cold ESP and the FGD unit are designed-
for sufficient dust removal.
  Low-temperature catalysts have been
used for 200-250°C gases such as that
produced by coke ovens, as shown in
system E of Figure 1. Since ammonium
bisulfate deposits on the catalyst at these
low temperatures, the catalyst requires
occasional heating to 400°Cto remove the
bisulfate.
  When wet FGD is applied downstream
of SCR or SNR, the ammonia present in
the reactor outlet is caught by the FGD
system and goes into the wastewater. In
some cases it may be necessary to use the
activated sludge process to  remove am-
monia from the wastewater.

Cost of NOX Abatement for
Stationary Sources
  The investment cost for a combustion
modification system is shown in Table 3.
Costs range from ¥400* to 8007 Mm3 of
flue gasor¥1,200-2,400/kW for 55-70%
reduction  using  a combined Iow-N0x
burner, staged combustion, and flue-gas
recirculation system.
  SCR  costs for new 700 MW gas-, oil-,
and coal-fired utility boilers are shown in
Table 4. For cost estimation purposes, it
was assumed that flue gases leaving the
boiler economizer at 330-400°C are treated
in two  equal-size reactors in parallel and
that unreacted NH% is kept below 5 ppm.
The investment cost for 80% IMOX removal
is about ¥2,500/kW for gas, ¥4,100-
6,200/kW for oil and ¥6,700-8,400/kW
for coal. The cost differences are due to
the varying  amounts of catalyst required.
For example, a small amount of a very
active catalyst is used for  gas streams
while a larger amount of a less active
catalyst which is resistant to SOX and dust
erosion is used for dirty flue gas (oil or coal
streams). Compared with 80% removal,
90% removal costs 1 5% more for gas, 25-
30% more for oil, and 30% more for coal.
The investment cost of an SCR system for
an existing boiler is 10-50% more than for
a new boiler.
B

370

sc/?

370

AU


150

ESP

-LA
Stack
           370
SCR
370

AH
                                             150
                                                       100
                                                             370
           370

AH
150


ESP
150
	 fc»


FGD
\



•







H
w

SCR
B
370

Hot
ESP
                       370
                                                       Heater
             Electrostatic Precipitator
Figure  1.   SCR and FGD system  arrangements in use in Japan. (Numbers indicate gas
           temperature in °CJ
Table 3.   CM Investment Cost

    Method              NOX removal, %     ¥/Nm3
                           ¥/kW
                          $/kWa
Low-NOx Burner
Combined System1'
20-40
50-70
100-200
400-800
300-600
1200-2400
1.2-2.4
4.8-9.6
(*) $1 =¥250.
a$1 =¥250.
hLow-NOx burner, staged combustion, and flue gas recirculation.


  The dirtier the gas, the shorter the life of    moved is lower with NGyrich gas.  The
the catalyst  Therefore,  the annualized    cost per pound for 80% removal is 10-1 7
SCR cosi/kWhr is  higher when SCR is    percent lower than the cost for 90% re-
used with dirty gas. On the other hand, the    moval.  NOX removal of 90% with a low
annualized  cost per  pound of NOX re-    level of unreacted NH3 (about 5 ppm) is

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   Table 4.    SCR Cost for 700 MW New Boiler (1981 Cost) (70% Boiler Utilization 4.292.000 MWhr/yr)
Fuel
Inlet NOX, ppm
Catalyst
Type
Cost lO6*/™3
Life, years
NOX Removal, percent
Investment Cost8,
1000 */kW
Annual/zed cost*,
¥/kWhr
Low-S High-S Low-S High-S High-S
Gas Oil Oil Coal Coal Coal
60 100 200 300 300 600
Pellet Honeycomb Honeycomb Honeycomb Honeycomb Honeycomb
3.0 3.3 3.3 3.5 3.5 3.5
43 3 2 2 2
80 90 80 90 80 90 80 90 80 90 80 90
2.47 2.80 4.13 5.11 6.23 7.93 6.69 8.51 7.26 9.10 8.44 10.7t
0.17 0.20 0.28 0.35 0.44 0.56 0.59 0.76 0.65 0.82 0.81 1.04
  "Including initial charge of catalyst civil engineering, and test operation.
  *Including 10% interest and 7 years depreciation.
   not easy to obtain with a large amount of
   gas from a utility boiler, because both gas
   velocity and NOX concentrations vary a-
   cross the duct at the reactor inlet
    The investment and annualized SCR
   costs for 80% S02 removal for coal-fired
   boilers are about one-third of those  for
   90% S02 removal using the wet lime/
   limestone FGD  process.   On the other
   hand, SCR is more expensive than CM.
   Although the investment cost of SCR for a
   gas-fired boiler is similar to that of CM in
   the combined system (Table 3), the annuah
   ized cost of SCR  may be considerably
   higher than CM,  which has low operating
   costs.  Therefore, for NOX abatement, CM
   should be used  first  and SCR should be
   used in combination  with CM when CM
   alone is not sufficient to meet control
   regulations. One CM technique, flue gas
   recirculation, is relatively expensive and is
   not  highly efficient  for coal.   For this
   reason, flue gas  recirculation may not be
   useful when SCR is applied to coal-fired
   boilers.
    The costs of other FGT processes  are
   uncertain because they have not been
   used widely in  continuous  commercial
       operation.   However,  experience with
       Thermal DeNOx, a type of SNR used with
       an oil-fired utility boiler, indicates that its
       cost is about half that of SCR although the
       NOX removal efficiency is  also half  as
       much (40% versus 80%).
          Jumpei Ando is on the Faculty of Science and Engineering, Chuo University.
            Tokyo, Japan.
          J. David Mobley is the EPA Project Officer (see below).
          The complete report, entitled "NO* Abatement for Stationary Sources in Japan,"
            (Order No. PB 83-207 639; Cost: $37.00, subject to change) will be available
            only from:
                 National Technical Information Service
                 5285 Port Royal Road
                 Springfield, VA 22161
                  Telephone: 703-487-4650
          The EPA Project Officer can be contacted at:
                 Industrial Environmental Research Laboratory
                  U.S. Environmental Protection Agency
                 Research Triangle Park, NC 27711
United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
Postage and
Fees Paid
Environmental
Protection
Agency
EPA 335
Official Business
Penalty for Private Use $300
    '  PSc  £0NX°lIZ?ROTECTlON  AGENCY

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