United States Environmental Protection Agency Industrial Environmental Research Laboratory Research Triangle Park NC 27711 Research and Development EPA-600/S7-84-094 Nov. 1984 Project Summary Characterization of Emissions from the Combustion of Wood and Alternative Fuels in a Residential Woodstove R. S. Truesdale, K. L. Mack, J. B. White, K. E. Leese, and J. G. Cleland This study was undertaken to com- pare the emissions from the combustion of alternative fuels to those from wood in a residential woodstove, and to check the effects of woodstove operating parameters on combustion emissions. Overall, oak wood is the best fuel tested, considering both emissions and stove operation. Compressed wood logs with binders and bituminous coal produce the highest emissions of SO2, particu- late, and NO,. Compressed wood logs without binders and treated lumber produce the highest PAH emissions. Important parameters affecting CO emission levels are fuel structure and, to a lesser degree, combustion air flow. SO2 emission levels are related directly to fuel sulfur content. NO, emissions are controlled by fuel nitrogen content and combustion air flow rate. Organic emissions are affected by fuel consump- tion rate, fuel structure, and amount of air through the stove. PAH formation is affected by combustion airflow, firebox temperature, and fuel structure. Bio- assay results indicate the presence of both mutagens and promutagens in the organic extracts of flue gas samples from both wood and coal combustion tests. 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 docu- mented in a separate report of the same title (see Project Report ordering infor- mation at back). Introduction The purpose of this study is to measure the emissions from the residential com- bustion of alternative fuels to wood, including coal, in a conventional wood- stove. Fuels tested include compressed wood, treated wood, newspapers, com- mercially available paper logs, and peat, in addition to untreated oak wood and bituminous coal. Pollutants including particulates, SO,, NOX, CO, PAH, organics, and benzo(a)pyrene were measured during the course of this study for the alternative fuels tested, and their emis- sion levels are compared to those from wood combustion. The effects of the stove operation parameters on emission levels of these pollutants are also con- sidered. This information should be useful in estimating the overall effect of these emissionsfrom residential solid fuel units on ambient air quality. Procedure During the planning phase of this project, eight fuels were chosen as likely alternatives to wood for use in residential combustion units. Dry oak wood wasalso tested so that emissions from alternative fuels could be compared to it. The alterna- tive fuels chosen were coal (both bitumi- nous and anthracite), peat, newspaper logs, cardboard logs, compressed wood- chip logs (both with and without binders). ------- and pine lumber pressure-treated with copper compounds to retard rot. The woodstove used in this study was free-standing and air-jacketed, with a simple open firebox. Originally designed as a fireplace insert, this type of stove is being installed in increasing numbers of new homes. The stove utilizes forced air circulation through the air jacket to con- vect heat into the room. Two successful runs were performed for each fuel except for anthracite coal, which was not successfully burned in the stove chosen for this study. Two tests were also carried out using split and round dry oak. These tests were used as a baseline for comparison to tests with other fuels. Temperature was measured during each run by several thermocouples: in the firebox and the stack, at the air jacket blower inputs and outputs, andinthetest room (ambient). Temperature data and certain gas data were automatically recorded by the online DEC PDP-1100 computer. An RTI-designed turbine meter (vane anemometer) was used for continu- ous flow measurements of the stack flow during each test. Stack gas composition was continu- ously monitored during the tests. Carbon monoxide, carbon dioxide, and methane were analyzed using infrared detectors. Nitrogen oxides (NO,) were measured using a photolummescent detector. Sul- fur dioxide (SO2) was measured using a photometric detector. In addition to con- tinuous gas analysis, gas bulb samples were also taken and analyzed by gas chromatography for total organic carbon. A whole-test-integrated sample of poly- cyclic organic matter and other organic emissions was collected by a modified Method 5 sampling train similar to the one described in the trial protocol. The train was assembled and checked out according to a test protocol developed to meet RTI's situation as well as to incor- porate the trial protocol. Mass emissions were collected over a 45 to 1 20 minute interval depending on the volume of sample required for analysis. Modified Method 5 samples which were analyzed for organics include: probe wash (CH2CI2 + CH2OH), filter, condenser and XAD module wash (CH2CI2), XAD-2 adsorbent, condensate catch, and im- pinger water. These samples were ex- tracted using an EPA procedure. Each test produced two samples: one was the concentrated extract of the XAD and particulate; and the other was the extract of the aqueous impinger solutions and the aqueous condensate. Organics analyses were performed separately on the two types of concen- trated samples. Total organics with a boiling point of 100 to 300°C were determined by total chromatographable organics (TCO). Organics with a boiling point above 300°C were determined by a gravimetric technique. Glass capillary gas chromatography (GC2) was used to determine PAH con- centrations in the modified Method 5 sample extracts. PAH analyses were performed separately on the two samples described previously. PAH-spiked sam- ples were used to identify PAHs in the unspiked samples. PAH concentrations were quantified using an internal stand- ard. GC/MS was used to confirm GC2 identifications for selected samples. In addition to GC2 analysis, a PAH sensitized fluorescence spot test was used to screen the XAD extract, con- denser and probe wash, and m the methylene chloride extract from the aqueous impingers and condensate sam- ples for the presence of PAHs. Both original and concentrated extracts were tested. To properly compare the emissions of the alternative fuels tested, it was neces- sary to sample only at steady-state stove operating conditions. Start-up and shut- down conditions were too variable for reproducible testing. Steady-state condi- tions were chosen to approximate condi- tions the typical stove owner would achieve for most of the stove's operation. Results and Discussion Comparisons of the emission factors of the fuels tested are given a figure for each pollutant. Emission rates in grams per hour and emission factors in grams per kilogram of fuel consumed are graphed in each figure. Particulate—Particulate emission re- sults for the eight fuels successfully tested are given in Figure 1. This figure shows that the fuels may be ranked by particulate emissions as follows (highest to lowest): 1. Compressed wood-chip logs with binders (CWB) 2. Bituminous coal (BC) 3. Newspaper logs (N) 4. Treated Lumber (TW) 5. Peat(P) 6. Compressed wood-chip logs (no binders) (CW) 7. Cardboard logs (C) 8. Wood (W) Sulfur Dioxide (SOg)—Figure 2 gives SO2 emission factors for the fuels tested. The eight fuels ranked as follows with regard to sulfur emissions (highest to lowest): 1. Bituminous coal 2. Compressed wood-chip logs with binders 3. Peat 75- 5- •n Jl g/kg fuel consumed Jl 40 30 -20 W CW CWB C Figure 1. Emission factors: particulate. BC ------- 8- 6 4- 2- rfl ^ B p/*0 foe/ consumed • 1 7.30 ft g/hr 1 1 Jl 1 <^i r^ ' 39.32 24 •22 20 18 16 14 •12 10 •8 6 •4 •2 X Ol W CW* CWB 'Factors based on single test. Figure 2. Emission factors' S 4. Cardboard logs 5. Wood 6. Compressed wood-chip logs (no binders) 7. Treated lumber 8. Newspaper logs SO2 emissions varied directly with fuel sulfur content. Nitrogen Oxides (NOJ—NOX emission factors are shown in Figure 3. Two rank- ings of fuel by NO, emissions are possible. First, considering NOX emission rates (g/hr), the fuels may be ranked as follows (highest to lowest): 1. Peat 2. Compressed wood-chip logs with binders 3. Bituminous coal 4. Wood 5. Compressed wood-chip logs (no binders) 6. Cardboard logs 7. Newspaper logs 8. Treated logs Considering NO, emission factors(g/kg fuel consumed), the fuels may be ranked as follows (highest to lowest): /v* TW* BC 1. Compressed wood-chip logs with binders 2. Bituminous coal 3. Peat 4. Wood 5. Newspaper logs 6. Cardboard logs 7a. Treated wood (same level as 7b) 7b. Compressed wood-chip logs (no binders) The difference in ranking between g/hr and g/kg emission factors is due to differ- ence in fuel consumption rates. Higher heating value fuels (BC and CWB) have low fuel consumption rates because less fuel has to be burned to produce a unit heat output. Two factors were found to influence NO, emission magnitude: fuel nitrogen content and stack gas flow rate. Fuel nitrogen content was judged to be the most important factor affecting NOX emissions from the combustion of these fuels. Carbon Monoxide (CO)—CO emission factors are given in Figure 4. CO emis- sions for the various fuels tested did not vary as much as with the previously discussed pollutants. The ranking of fuels according to CO emission factors (g/kg fuel consumed) is as follows (highest to lowest): 1. Newspaper logs 2. Compressed wood-chip logs with binders 3. Peat 4. Bituminous coal 5. Cardboard logs 6. Compressed wood-chip logs (no binders) 5- 4- 3- 01 X O) 2- 1- ff/^ff fuel consumed , I 12 W IV CW CWB C N Figure 3. Emission factors: fl/O,. TW BC ------- 7. Treated lumber 8. Wood Ranking of fuels according to CO emis- sion rates (g/hr) is as follows (highest to lowest): 1. Newspaper logs 2. Compressed wood-chip logs (no binders) 3. Peat 4. Cardboard logs 5. Compressed wood-chip logs with binders 6. Treated lumber 7. Wood 8. Bituminous coal Reasons for the change in ranking between emission factors (g/kg) and emission rates (g/hr) are related to fuel consumption rates and fuel heating values as discussed earlier for N0« emis- sions. CO emission levels could not be suc- cessfully correlated with stove operating parameters, including stack flow rates, firebox temperatures, stack temperatures, fuel consumption rate, and heat output. The physical structure of the fuels tested probably is the major factor affecting CO emissions: compressed man-made fuels have higher CO emissions than the naturally formed fuels (wood and coal). Results from duplicate tests for each fuel suggest that combustion air flow also affects CO emissions: reduced air flow leads to increased emissions. Organics—Results from total chromat- ographical organics and gravimetric analyses indicated that total organic emissions in the flue gas were similar for all fuels except N andP, which had higher organic emission factors. This is some- what surprising since N had the lowest PAH emission factors. BC, with organic emissions comparable to most other fuels, had the highest proportional contribution of heavy organics. Polynuclear Aromatic Hydrocarbons (PAH)—?M\ formation was affected by combustion air flow, firebox temperature, and fuel structure. Composite structured fuels had higher PAH formation except for N which, in contrast to high total organic emissions, had very low emis- sions of heavier PAHs. It was concluded that, during the tests with N, firebox temperatures were too low for extensive cyclization reactions leading to PAH formation. Other composite fuels had relatively high PAH production rates: 700- 80 60 f 40 20 g/kg fuel consumed 300 200 h700 W CW CWB Figure 4. Emission factors: CO. N TW P BC 5- 4- n n w CW CWB N TW BC Figure 5. Emission factors, benzfajpyrene attributed to their structure, which limits the availability of air during combustion and creates starved air conditions favor- able to PAH production. Tests with TW also had relatively high levels of PAHs in the flue gas effluent stream: attributed to low air flow through the stove during these tests. W and BC had similar PAH emissions: BC emitted less PAHs than wood. PAH emissions from BC could possibly be pyrolysis products from the coal itself. Figure 5, a comparison of benz(a)pyrene (BaP) emission factors for eight fuels tested, shows that BaP emis- ------- sion factors are lowest for N. W and BC have similar levels. Other fuels had higher BaP emission factors probably due to burning characteristics which reduce air to the fuel (particulate fuels) or to very low air flow through the stove (TW). Bioassay—Method 5 sample extracts from one W combustion (W1) and one BC combustion test (BC1) were subjected to an Ames Salmonella mutagenicity assay to measure their mutagenic potential. The results of bioassay analysis suggest the presence of frameshift and base pair substitution mutagens in both samples. Both samples were highly mutagenic with TA98 and moderately mutagenic with TA100. Both samples demonstrated an increase in mutagenic activity with the addition of S9, a metabolic activator of promutagen compounds. Therefore, both samples contain direct-acting mutagens and promutagens. The BC combustion sample was more mutagenic than the W combustion sam- ple, based on the slope of the dose/ response curves in units of revertants/ mg of sample. Putting bioassay results on a revertants/kg of fuel consumed basis, the BC extract is more mutagenic than the W extract by a factor of two. Since emission factors (g/kg) for the PAHs analyzed in this report are only slightly higher for BC1 than f or W1, this suggests that compounds other than the 24 PAHs analyzed in this report may be contribu- ting to the mutagenicity of these samples. Conclusions 1. Overall oak wood (W) was the best fuel, considering both emissions and stove operation. Cardboard logs (C) were almost as good as W. Although they did emit more CO and PAHs than W, levels of these pollutants were lower than for most other fuels, and stove operation was easier with C than with other fuels. 2. Compressed wood logs with binders (CWB) and bituminous coal (BC) produced the highest emissions (g/kg fuel consumed) of S02, partic- ulate, and NO,. In addition, CWB emissions were high in CO and PAHs. 3. Compressed wood logs without binders (CW) were determined to be unsuitable for stove use on safety grounds. CW also emitted large amounts of CO and had the highest PAH emission rates of all fuels. 4. Treated wood (TW) should not be burned under any circumstances because of the presence of arsenic compounds which probably volatil- ize during combustion. Other stud- ies have shown that, in the com- bustion of chlorophenol-treated wood products, polychlorinated dibenzo-p-dioxins (PCDD) and poly- chlorinated dibenzofurans (PCDF) are emitted. 5. Peat (P) emissions had relatively high levels of NO*, SO2, CO, and PAHs. 6. Particulate matter from BC and CWB combustion was sooty and sticky. These fuels produced the highest particulate emission by far. Composite fuels (CW, C, P, news- paper (N)) produced particulate emissions higher than those of W. High particulate levels for N and TW were largely attributable to condensed organics. 7. Important parameters affecting CO emission levels were fuel structure and, to a lesser degree, combustion air flow. Fuels with a man-made, compressed particulate structure (CW, CWB, C, P) and N had high CO emissions because their structure inhibited air flow to the combustion zone. W, TW, and BC had the lowest CO emissions: these fuels would shrink and crack when burned, permitting sufficient air to reach the burning fuel. Results from dupli- cate tests for each fuel suggest that air flow through the stove is also a factor affecting CO emissions: re- duced air flow leads to increased emissions. 8. S02emission levels could be related to fuel sulfur content: higher fuel sulfur content causes higher S02 emissions. SO2 emissions were at levels of environmental concern only for P, BC, and CWB. 9. NOX emissions were controlled by fuel nitrogen content and combus- tion air flow rate. High nitrogen content f uels (P and BC) had highest NO, emissions. Increased air flow through the stove also led to in- creased NO, emissions. NO, levels, generally low, were not as much of a concern as other pollutants. 10. Organic emission levels were com- parable for all fuels except P and N, which had high levels of organics in the flue gas effluent stream. Organic emissions were affected by fuel consu mption rate, fuel struc- ture, andamountof air through the stove. Higher fuel consumption sometimes led to increased organ- ics. Lowering air flow through the stove increased organic emissions. N had high organic emissions be- cause of their physical structure, which inhibited air from reaching the combustion zone leading to increased pyrolysis products. 11. PAH formation was affected by combustion airflow, firebox temper- ature, and fuel structure. Composite structured fuels had higher PAH formation except for N which, in contrast to high total organic emis- sions, had very low emissions of heavier PAHs. It was concluded that, during the tests with N, firebox temperatures were too low for extensive reactions leading to PAH formation. Other composite fuels had relatively high PAH production rates: attributed to their structure, which limits the availability of air during combustion and creates starved air conditions favorable to PAH production. Tests with TW also had relatively high levels of PAHs in the flue gas effluent stream: attrib- uted to low air flow through the stove during these tests. W and BC had similar PAH emissions, with BC emitting less PAHs than wood. PAH emissions from BC could possibly be pyrolysis products from the coal itself. 12. Bioassays on organic extracts from one W test and one BC test demon- strated the presence of both muta- gens and promutagens in the sample extracts. Organics from BC combustion were about twice as mutagenic as those from W com- bustiorf on a mutagenicity per unit mass of fuel consumed basis. ------- /?. S. Truesdale, K. L Mack, J. B. White, K. E. Leese, andJ. G. C lei and are with Research Triangle Institute, Research Triangle Park, NC 27709. Michael C. Osborne is the EPA Project Officer (see below). The complete report, entitled "Characterization of Emissions from the Combustion of Wood and Alternative Fuels in a Residential Woodstove," (Order No. PB 85-105 336; Cost: $14.50, subject to change) will be available only from: National Technical Information Service 5285 Port Royal Road Springfield, VA22161 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 irUSGPO: 1984—559-111/10722 ------- United States Environmental Protection Agency Center for Environmental Research Information Cincinnati OH 45268 BULK RATE POSTAGE & FEES PAID EPA PERMIT No. G-35 Official Business Penalty for Private Use $300 PS 0000129 4GENCV ------- |