United States Environmental Protection Agency Air and Energy Engineering Research Laboratory Research Triangle Park NC 27711 Research and Development EPA/600/S7-89/005 Feb. 1990 ve/EPA Project Summary Bench-Scale Studies to Identify Process Parameters Controlling Reburning with Pulverized Coal D. W. Pershing, M. P. Heap, and W. R. Seeker The report addresses the evaluation of a technology which is a combination of two technologies used to control the atmospheric emission of NOX by stationary sources: (1) combustion modification (controls flame temperature and maximizes fuel-rich residence time to minimize NOX formation); and (2) flue gas cleaning (uses a reducing agent with or without a catalyst to remove NOX from combustion products). The combined technology uses fuel as a reducing agent to remove NOX. The process (referred to as in-furnace NOX reduction, reburning, and staged fuel injection) can be applied to many types of combustion systems. In fact, reburning is the process which allows the "in-furnace NOX reduction" to take place. This Project Summary was devel- oped by EPA's Air and Energy Engineering Research Laboratory, Research Triangle Park, NC, to announce key findings of the research project that is fully documented in a separate report of the same title, (see Project Report ordering Information at back). Introduction This report summarizes the results of a small theoretical and experimental study which was undertaken as part of the EPA's Fundamental Combustion Research Program to investigate in- furnace NOX reduction (reburning). In simple terms, the reburning concept involves the use of a heat release zone (via staged fuel addition) to convert NO formed earlier in the main combustion zone into some form which will ultimately produce N2. The process takes place in two discrete zones. 1. NO Reduction Zone. Here fuel is added to produce CH radicals which reduce part of the NO from the main combustion zone to N2, HCN, and NH3. 2. X/V Oxidation Zone. Here the final combustion air is added and a percentage of the total fixed nitrogen (TFN) pool (HCN + NO + NH3) and char nitrogen (if any) are oxidized to NO as the remaining fuel fragments burn to C02 and H20). Thus, NO can produce N2 in both zones and the key to reburning is to provide the species and temperatures which allow this to happen. The first zone forms N2 but also converts NO into species which can also be converted to N2 in the second zone. Data Available Figure 1 shows data obtained with coal firing, demonstrating the overall potential of the reburning concept (referred to as Mitsubishi Advanced Combustion Technology, or MACT). This figure also shows data obtained in the boiler simulator furnace (BSF) at Energy and Environmental Research Corporation. Both sets of data indicate that it is possible to achieve extremely low levels (50 ppm NOX at 6% 02) under ideal combustion conditions; in general, it has been possible to reproduce the Japanese results under similar test conditions in the U.S. However, the application of reburning to large-scale commercial systems in the U.S., burning a wide ------- range of bituminous and low-rank coals, is not as simple as Figure 1 suggests. In the reburning process NO can produce N2 in both zones and, to optimize the process, it is necessary to provide the species and temperatures which maxi- mize the rate of N2 formation. Some NO is reduced to N2 in the first zone, but the remaining NO either remains as NO or is converted into species which are capable of being reoxidized in the second stage. To investigate the optimization and application of reburning, experimental studies were conducted in two facilities: a 5.7 cm ID, 7.38 MJ/hr (2kW), back-fired, laboratory reactor firing doped gaseous fuels and a 15.2 cm ID, 73.8 MJ/hr (21 kW), tunnel furnace firing pulverized coal. The reburning fuels used in this investigation included propane, North Dakota lignite, bituminous coals from Utah and Alabama, and Australian coal. Conclusions The principal conclusions of the work relate to both the NO reduction zone and the XN oxidation zone. NO Reduction Zone 1. The optimum rich-zone stoichio- metry (SR2) is approximately 0.9 because of the tradeoff between NO reduction and increased concentration of easily oxidizable N species. Figure 2 compares the data from several sources and attests to the consistency of the overall conclusion. At stoichio- metries leaner than 0.9, the initial NO is not reduced as effectively perhaps because of a lack of CH radicals. At rich-zone stoichio- metries below approximately 0.9, large amounts of TFN species (particularly HCN and NH3) are produced and ultimately oxidized to NO in the final stage. As Figure 2 indicates, this problem is greatly enhanced with coal, where the reburning fuel nitrogen becomes more significant as additional reburning fuel is added. 2. The primary zone stoichiometry (SR,) has little influence on the exhaust NO at the optimum reburning conditions. Increasing SR1 only slightly decreases effectiveness of the reburr concept in spite of a large inc« in the available reactive nitroge the rich zone (due to increz reburning fuel). 3. The nitrogen content of reburning fuel has only a s effect on the reburning efficienc optimum combustion condith but at lower rich-zone stoic metric ratios, it can be of IT importance. Figure 3 shows obtained with doped prop flames and indicates that at zone stoichiometries be approximately 0.8, the nitre content of the reburning fuel gn influences the effectiveness of reburning concept. This ii particular importance becaus large-scale utility system w inevitably have a distributioi rich-zone stoichiometries ac the combustion chamber in reburning zone. 4. The effectiveness of rebur depends strongly on 250 200 150 o § too I o 3 50 Rate of Combustion: - Fuel: No. of Burner Units: BSF Data H50kg/h Taiheiyo Coal 3 (Stages) x 4 (Corners) MACT = Mitsubishi Advanced Combustion Technology BSF = Boiler Simulator Furnace \ I I i I I 0 1 23456 O2 Concentration in Exhaust Gas, percent Figure 1. NOX removal effect for coal firing. ------- ID Q. 90 00 70 60 50 40 30 20 10 Model Prediction (500 ppm) Wendt (WOO ppm = NO/, Secondary Reduction Only) _.._ Takahashi et al. (Gas Phase, 100 ppm NO) EER Gas-Phase Data (540 ppm, EER Propane/Beulah Bench Scale (633 ppm) I _ I _ I _ I _ I 0.60 0.70 0.80 0.90 T.O Stoichiometry of the NO Reduction Zone Figure 2. Effectiveness of reburmng-subscale data. 1.1 1.2 relationship of the initial NO concentration to the amount of reburning fuel nitrogen added to achieve an overall rich-zone Stoichiometry of 0.9. Figure 4 shows that, even with optimum combustion conditions at low initial NO levels, reburning may actually increase exhaust NO emissions. With an initial NO level of approximately 150 ppm and a typical coal as the reburning fuel, the reactive nitrogen available in the rich zone increases almost fivefold when the reburning fuel is added to acheive an overall Stoichiometry of 0.9. 5. Coal composition is important because it influences char burnout, the initial NO level, and the freburning fuel nitrogen content and speciation. Many coals commonly used in the U.S. for power generation may prove to be relatively unsuitable for reburning, particularly in retrofit applications, because it will not be possible to effectively burn out the coal char in the available time. XN Oxidation Zone 1. The TXN (total fixed nitrogen, including char N) conversion depends on the XN speciation, the XN concentration, the hydrocartbon content at the rich-zone exhaust, and the thermal environment. 2. Low XN conversions can be achieved by tailoring the temperature profile to obtain selevtive reduction of NO by NHj species in the final, oxygen rich stage. Figure 5 summarizes the results obtained in the tunnel furnace and shows the dramatic influence of thermal environment on the effectiveness of the reburning concept for two initial NO levels. This effect is believed to be directly related to a large decrease in the TFN conversion in the final stage of the reburning process. In summary, the overall processes controlling the reburning phenomena have been relatively well-identified and characterized. Although the elementary reactions are not fully understood, the key parameters have been identified and the overall mechanisms defined. Further work could define the influence of mixing rates and establish the potential impacts of applying reburning to boilers and furnaces. ------- (NO)., = 633 ppm 170 160 150 140 1 130 I 120 \ 1W S. 700 90 80 70 60 50 40. 0.6 0.7 0.8 SR2 0.9 1.0 Figure 3. Effect of SR2 and reburning-fuel nitrogen content (tunnel furnace). ------- * NHj. N * 1.04% 120 a 80 40 20 SR, = 1.1 SR2 = 09 SR3 = 1.2S o- I 200 400 600 800 1000 1200 (NO)p, ppm Figure 4. Influence of returning fuel type and primary NO level. CjHg/Seu/an 2400 2600 2800 3000 600 500 400 300 200 too I I T _ Open - Normal Closed - Secondary Cooling SR, = 1.1 SR3 = 1.25 0.6 0.7 0.8 0.9 SR2 Figure 5. Effect of secondary cooling on exhaust NO emissions. 1.0 1.1 ------- D. W. Pershing, M. P. Heap, and W. R. Seeker are with Energy and Environmental Research Corp., Irvine, CA 92714-4190. W. Steven Lanier is the EPA Project Officer (see below). The complete report, entitled "Bench-Scale Studies to Identify Process Parameters Controlling Returning with Pulverized Coal," (Order No. PB 89-200 81 Oi'AS; Cost $21.95, 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: Air and Energy Engineering 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 Official Business Penalty for Private Use $300 EPA/600/S7-89/005 US.OFFICIAL MAIL" O.S.POSlAGc ? 0 3 5 = CHICAGO ------- |