3506B24 Final Report
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- Figure 47
- 7 CONCLUSIONS AND OUTLOOK
- 8 REFERENCES
Figure 46: Prescribed burning area (acres) and location (direction from OLC) with wind direction (in deg N), CO (ppbv), and OC mass fraction (per mil) measured at OLC (top); PM2.5 mass and composition (center); and speciated POC from HVS samples taken at OLC during the burn events in late April. The numbers in the center panel represent the OM/OC ratio from the mass closure approach. Numbers in the bottom panel denote the size of the burn areas in acres. 6.6.4 Source Apportionment from CMB for February case As mentioned in the case discussion above, contributions from primary PM2.5 emissions of various source categories similar to the ones used in the VOC source apportionment were computed for the February samples using the CMB7.0 software developed by Watson et al. [1990]. In a preliminary approach, source profiles were established from literature values for the categories 1) diesel exhaust, 2) gasoline exhaust, 3) wood combustion, and 4) vegetative detritus and entered into the multi-linear regression model. The results are presented graphically in Figure 47 and in Table 30 for numerical reference. The “Other OC” category may contain minor contributions from meat cooking sources but is largely unassignable to any specific sources, and can be attributed predominantly to products of secondary atmospheric processes such as SOA. Aside from this latter category, wood combustion is the major source at the OLC site, and its contribution changed over time during the burning. The flaming stage of the prescribed burning of total 937 acres at ca. 28km to the east, occurred on the 5th between 1200 and 1700 EST, although under strong northwesterly flow. The wind weakened and veered over north to easterly directions during the subsequent smoldering and potential plume impact stages of the late night and early morning hours. The Hi-Vol and PCM samples were taken at OLC during a pre-burn (background) period on February 1st, and during several 5 h sampling periods, separated by the afternoon flaming stage (12-1700), the evening smoldering stage (17-2200), the nocturnal post-burn potential plume impact stages (22-0300, and 03-0800), and a post-burn morning “traffic rush hour” stage (08-1300). Average meteorological quantities and air pollutant concentrations (and ratios) for this burn event indicated OLC being inluenced by strong north-westerly flow during the flaming stage with relatively low loadings of primary pollutants NO (NOy) and CO (see above case description). This agrees with the relatively low OC contribution from wood combustion sources found in the CMB for the flaming stage sample in Fig. 47, compared to the later samples. Even during the smoldering stage, the OLC site was still under mostly northerly flow. Higher loadings in primary pollutants as well as higher CO/NOy ratios appeared only during the calmer post-burn indirect plume impact stages, especially between 2200 and 0300 EST, with clear, although weak easterly component flow. The sample taken between 0800 and 1300 on the 6th, shows a significantly enhanced contribution from diesel exhaust, indicative of the likely influence from local traffic sources during the morning rush hour period. Note that Fort Benning’s work force consists of more than 15,000 people, a large fraction of whom commute to work daily. But the OLC also receives visitors on a regular basis, and especially during the school year, buses frequently arrive in the morning with school classes from the Chattahoochee and neighboring counties. The PCM data from this event (see above) indicated already a significantly higher PM2.5 mass loading of organic compounds after the active (flaming) burn period, beginning with the “smoldering” phase at 1700, while the sulfate mass fraction was clearly decreasing. Also, the preliminary POC data from GC/MS analysis showed elevated levels of the biomass burning markers levoglucosan and resin acids as the main contributors to the identified organic mass in the post-burn samples, which was confirmed by the large contribution from the wood smoke source after application of the CMB, again stressing the dominance of the prescribed burning to the overall fine PM loading. Although the primary indicators (CO, NOy, PM2.5) did originally not suggest a direct impact of the prescribed burning plume, a significant contribution to the fine PM mass was detected in a more dilute indirect and probably more regional impact. Uncertainty in this interpretation is founded by the wood combustion profile used in this initial CMB model run. These profiles were almost exclusively determined in laboratory environments, which cannot accurately reproduce the conditions that are encounterd in real world prescribed burning applications. 
Figure 47: Source contributions to organic carbon (OC) in PM2.5 at the OLC site outside Fort Benning, GA, for samples taken on February 1, 5 and 6. Table 30: Absolute (top) and relative (bottom) source contribution to organic carbon (OC).
7 CONCLUSIONS AND OUTLOOK This study was motivated by the immenent need to develop an effective and efficient strategy that provides the ecological benefits afforded by prescribed burning without compromising an area’s ability to meet clean air goals. The main questions addressed here were: 1) To what extent does prescribed burning actually affect local and regional air quality? 2) What types of pollutants are emitted and in what quantities (absolute and relative to other sources)? 3) In what way are these pollutants physically and chemically transformed in the atmosphere? and 4) How do different environmental conditions and burning practices affect the pollutant loads and transformation pathways? Semi-continuous PM2.5 mass concentration measurements made at a research monitoring station, established near Fort Benning, Georgia at the Oxbow Meadows Environmental Learning Center (OLC) revealed that the 24-h average National Ambient Air Quality Standard (NAAQS) for PM2.5, which is 65 µg m-3, was exceeded on five different days during a three-week period in the fall of 2001. The OLC site was operated as part of the Georgia Environmental Protection Division (GA-EPD) sponsored Fall-line Air Quality Study (FAQS, see http://cure.eas.gatech.edu/faqs/index.html for more details). Among all FAQS monitoring network sites, OLC was the only one where these exceedances occurred, and they contributed to an annual arithmetic mean of 16.9 μg m-3, which is 1.9 μg m-3 above the annual PM2.5 NAAQS. Exclusion of these five exceedances yields an annual mean of 14.4 μg m-3, clearly below the NAAQS, achieving attainment. These occurrences could be undoubtedly linked to prescribed burn activities on the military installation and caused the above questions to be raised. Analysis of the conditions leading to these locally confined exceedances showed that fine PM concentration is most sensitive to wind speed and atmospheric stability, leading to PM accumulation under calm conditions especially associated with nocturnal inversions. The relatively high uncertainties in wind direction measurements and plume trajectory calculations under such calm conditions, complicate the prediction of boundary layer mixing heights that effectively promote dilution of fine PM emitted near the ground at day, or on the other hand trap PM that are being emitted at night. The analysis also demonstrated that under stagnant atmospheric conditions smoldering fires represent a significant source for additional local air pollution extending continued emissions into the lower atmosphere over the next day or more, until the weather pattern changes significantly. The fine PM mass and the organics mass fractions increased as prescribed burns were conducted later in spring and early summer, suggesting to minimize burns in the warmer, photo-chemically more active months. The abundance of O3, indicating the oxidative capacity of the lower atmosphere, was seen low in March and May, corresponding to above normal precipitation across Georgia. The much drier April saw the highest maximum O3 levels, and hence allowed the highest SOA contributions to the observed fine PM mass concentrations. VOC emission profiles for both flaming and smoldering phases were similar for burns at Forts Benning and Gordon, with the only significant differences in α-, and ß-pinene and i-pentane. Ranking the VOC emissions according to their reactivity with OH, emphasized the importance, with respect to ozone formation, of the biogenic VOC emitted in excess during both burn phases. VOC that are potentially involved in the formation of SOA, e.g. the main aromatic species benzene, toluene, and xylenes, were emitted by prescribed burns in quantities similar to those of county-wide emissions from mobile sources (on road cars and trucks). Among ten aromatic species investigated, toluene was estimated to be the major SOA precursor species for the flaming phase, whereas the xylenes became the dominant precursor for potential SOA formation from smoldering emissions. VOC source apportionment using a chemical mass balance (CMB) method, showed diesel exhaust, gasoline exhaust, evaporative gasoline, refinery fugitive, primers and enamel, biogenic, and prescribed burns all contributing to VOC concentrations at the OLC receptor site. Prescribed burning reached a peak of 15% of the total VOC late at night, suggesting an important influence by the same meteorological processes (nocturnal temperature inversion, BL stratification and local cool-air pooling) that were found to have driven the local [PM2.5] exceedances in the fall 2001 case. Emissions of tracers can vastly vary with combustion temperature, fuel type and moisture. More importantly also, the laboratory experiments cannot simulate the response of the ecosystem surrounding a prescribed fire. For example, the soil’s top horizon will respond vividely to the heat generated by the combusting fuel on top of it, and release semi-volatile compounds from dead plant matter and microbes. In addition, the surrounding plants that are photsynthetically active will respond to the fire’s heat by excess transpiration through their stomates, thus releasing volatile compounds such as isoprene and terpenes in excess amounts, as well as less volatile, or semi-volatile compounds. Both groups play important roles in producing new PM via secondary pathways in the atmosphere by either gas-to-particle conversion and partitioning (e.g. terpene oxidation) or heterogeneous reactions involving hydration and polymerization processes of organics, especially after excessive flora transpiration and subsequent condensation during rapid cool down of the fresh plume. Specific tracers for biomass burning can be used to identify the contributions from the burning of different biomass materials. Such measurements can be used in molecular marker source apportionment models to quantitatively determine the impact of primary emissions from combustion sources on atmospheric PM concentrations. In order to further develop potential benefits for the public health and welfare of the State of Georgia in meeting air quality standards, and in response to the need for guidance in the development of a Smoke Management Plan for Georgia, the development of detailed source profiles for the specific prescribed burning activities on and around Georgia’s military installations is necessary. The GC/MS analysis method is limited to detect and quantify the less polar organics, explaining only a very small fraction (<10%) of the total organic mass. Hence, any source profile developed from GC/MS identified compounds remains an incomplete representation of the composition of organic compounds emitted by prescribed burning in reality. Colleagues at Georgia Tech have begun to investigate methods for broad classification of compounds based on solid phase extractions (SPE) followed by TOC analysis, which may provide unique insights into the sources of the organic aerosol, and also provide a means to simplify the complex chemistry for subsequent more detailed chemical analysis. The method broadly separates water-soluble OC (WSOC) into hydrophobic and hydrophilic components, where the hydrophobic fraction can be further divided into acidic, basic, and neutral components. The most dominant hydrophobic acidic WSOC species are humic and fulvic acid (referred to as humic-like-substances, HULIS), which are suspected to be also emitted in significant quantities from open biomass burning. The results of the study here point to a significant emission of oxygenated POC by prescribed burning indicated by relatively high OM/OC ratios early in the season. Due to the limitations of the GC/MS methods to measure these more polar compounds, other techniques have to be developed and utilized. The development of such analysis methods such as Proton Nuclear Magnetic Resonance (1HNMR), High Pressure Liquid Chromatography or Electro-spray Ionization coupled with Mass Spectrometry (HPLC-TOF/MS, ESI/MS) is the focus of many research groups in the scientific community, and are currently being tested at Georgia Tech on the various separated WSOC fractions to further chemically characterize the WSOC. In order to link these new methods to the prescribed burning issues, a suite of comprehensive samples from various burn sources and ambient receptor sites have to be collected and analyzed accordingly. In a Phase I continuation of this project here, first smoke samples were collected from prescribed burning sources at Forts Gordon and Benning in a brief field intensive in April 2004, and analyzed for various aerosol constituents. Preliminary analysis of these samples show a relatively large variability in composition and magnitude of primary POC emitted. Further analyses of these source samples applying new technologies like the above mentioned, will allow a much more accurate determination of the POC emissions profile for prescribed burning in Georgia. Subsequently, ambient PM2.5 samples will be able to undergo a source apportionment analysis with more accurate determination of the contributions from prescribed burning. The sampling of more plumes is necessary to capture the spatial and temporal variability of POC emissions, and to establish region-specific emission profiles for different parts of the season. Further POC speciation at collocated PM2.5 network monitoring sites will allow to link routinely monitored air quality data with specific source impacts from prescribed burning sources. 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