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- ------- 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 ------- 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 ------- 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 ------- |