United States Environmental Protection Agency Atmospheric Research and Exposure Assessment Laboratory Research Triangle Park, NC 27711 Research and Development EPA/600/S3-90/058 Sept. 1990 &EPA Project Summary An Assessment of Atmospheric Exposure and Deposition to High Elevation Forests in the Eastern United States Volker A Mohnen The spruce-fir forests in the higher elevations of the Appalachian Mountains from North Carolina to Maine are showing visible symptoms of injury and increased mortality. Concern has been raised that exposure to and deposition of atmospheric pollutants might play a role in this decline. The Mountain Cloud Chemistry Project (MGCP) sponsored by the U.S. Environmental Protection Agency (EPA) and the National Acid Precipitation Assessment Program (NAPAP) has studied the exposure and deposition of atmospheric constituents to these forests. Atmospheric pollution is deposited to the forest in a number of forms, cloud water interception represents a major deposition pattern and may exceed deposition by precipitation and gases. The full report provides estimates of cloud, precipitation and dry deposition to the spruce-fir forests at the MCCP sites. This Project Summary was developed by EPA's Atmospheric Research and Exposure Assessment 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 is the third in a series of annual summaries of research on the exposure and deposition of airborne chemicals to forest canopies and the forest floor in eastern North America. The report is based on observations and model estimates of atmospheric deposition at the high elevation sites in the eastern United States The report is produced by the scientists in the Mountain Cloud Chemistry Program, a multi-year study of atmospheric chemistry and physics sponsored by the EPA. The MCCP has three primary objectives: (1) determine the elevational gradients in wet and dry deposition of pollutants and climate variables; (2) determine the relative significance of various deposition mechanisms to the fluxes of chemical species into and through forest canopies; (3) determine the frequency distributions of chemical, physical and climatic exposure. This report provides estimations of forest exposure to chemicals in air and cloud water and deposition to the forests from precipitation, wind blown clouds and by dry deposition mechanisms. Measurement methodology used provide data for these estimations, data sets and models used for deposition estimates are discussed in detail. Comparisons of deposition are made between southern and northern MCCP sites. Elevation gradients in exposure and deposition are also discussed. Two models are used to estimate cloud water and chemical deposition flux. One model was developed by Lovett and modified by Mueller. This model is designed for use with spruce-fir forest canopies. The other model was ------- developed by Krovetz for use with the deciduous canopy at the Shenandoah MGCP site. The model used to estimate dry deposition is the inferential or "big leaf" model. Since this model was originally developed for flat terrain and the model has not been fully characterized for mountainous regions, deposition estimates reported here reflect these uncertainties. Technical Approach Resource and logistical considerations dictate that measurements of inputs to high elevation forests in eastern North America can be performed at only a limited number of sites where proper access and facilities are available. In order to meet the needs of the project, five high elevation sites have been selected from 45°N to 35°N to be representative of the geographic and meteorological variability in this large region. This coverage has been augmented by the addition of a low level site (Howland, ME) to allow evaluation of the impact of elevational gradient forest types and enhance geographical coverage. The research/monitoring sites associated with MGCP are Howland Forest, ME, Mt. Moosilauke, NH, Whiteface Mtn., NY, Shenandoah, VA, Whitetop, VA, and Mt. Mitchell, NC. Site specific measurements of cloud and rain water, of gaseous sulfur and nitrogen compounds, and of ozone and hydrogen peroxide are sampled hourly or are directly converted into hourly concentration values. In the case of filterpack measurements, samples are integrated over a week's time. These concentration values then represent the primary exposure parameters. The concentration of pollutants and the associated meteorological conditions are needed to provide estimates of deposition by precipitation,clouds, and gases. Results Deposition of Pollutant Ions in Precipitation Wet deposition of pollutants was estimated for the 1987/88 growing season at the MGCP sites using standard National Acid Deposition Program/National Trends Network (NADP/NTN) measurements of rainfall amounts and chemistry. The NADP sites selected to represent MGCP sites are Greenville, ME 09, Whiteface, NY 98, Hubbard Brook, NH 02, Big Meadows, VA 29, Whitetop, VA 28 and Clingmans Peak, NC 45. The growing season is longest at the Shenandoah and Howland sites, extending from early April at both locations to mid-November and early October, respectively. Mt. Mitchell and Whitetop Mountain have the next longest growing seasons, followed by Mt. Moosilauke and Whiteface with the shortest (June to early October). The wet deposition data are shown in Table 1 for S042- N03 and NH/ions in precipitation (not cloud). The data indicate that the most westerly sites in the north, Whiteface, NY and Moosilauke, NH, received greater wet deposition via precipitation than did the more northeasterly location in Maine. The southern sites showed slightly higher sulfate and nitrate wet deposition than the northern sites. Concentration and Deposition of Pollutants in Cloud Water The 1986-88 results for the five high elevation MGCP sites are summarized in Table 2 as overall chemical composition of cloud water samples from precipitating and non-precipitating clouds. The concentrations in non-precipitating clouds are significantly higher than in precipitating clouds. The differences in cloud water ion concentration between the sites is a result of sample location with regard to cloud base and synoptic weather type. The southern sites frequently are cloudy under the stable, warm sector synoptic type, while the northern sites experience cloudiness associated more frequently with frontal passage. Hence, any north-south differences in cloud water concentrations are likely related to cloud climatology including cloud base height. The importance of sample location in relation to height above cloud base can be demonstrated for Whiteface-1 (1483 m) and Whiteface-2 (1245 m). For simultaneously obtained cloud water samples, Table 3 shows the differences in the mean ion concentration observed for the two vertically separated sites.The substantial vertical gradient in cloud water concentration is mainly explained by increased dilution of precursor substances as liquid water increase with height above cloud base. In estimating cloud deposition to the forest canopy, MGCP uses an improved version of the 1984 Lovett Cloud Deposition Model (COM). Cloud impaction events at each MGCP site are classified according to meteorological conditions that prevail during each hour of the event A detailed analysis of cloud chemistry and meteorological variables (wind speed and liquid water content) has demonstrated the usefulness of this technique for uniquely characterizing conditions during events. In addition to synoptic classification, specific air trajectory directions computed within a given event type can further characterize event conditions. This technique is able to explain a major portion of the variance in the chemistry and meteorological data base, thereby allowing more complete growing season estimates of cloud deposition. Deposition estimates for MGCP sites can now be made for periods when data are incomplete as long as cloud frequency and event type can be determined. Event types are (1) pre-warm front, (2) NW sector of cyclone, (3) post- cold front, (4) warm sector of cyclone, (5) stationary front, (6) marine flow off Atlantic, (7) cutoff low in upper atmosphere, and (9) cap cloud. Cloud deposition estimates for each site are made by computing, for each subclass, the mean water deposition flux using the improved CDM and subclass wind speed and liquid water content. Best estimates of canopy structure are then used to calculate the gross (pre-evaporaiion) cloud water flux to specific forest canopies at each site. Most of the site-differences in cloud deposition can be explained on the basis of differences in canopy structure. Cloud deposition is found to be highly site specific. Despite an almost 2:1 advantage in cloud frequency, Whiteface Mountain mean deposition estimates for the growing season are generally lower than those for Moosilauke because of lower canopy surface area at the specific Whiteface site. Differences in cloud water deposition between the northern and southern sites are significant and likely caused by differences in such parameters as canopy structure, elevation above cloud base and synoptic meteorology. It is also interesting to note the annual changes in cloud water deposition as a result of changing meteorological conditions from year to year. Dry Deposition of Gases and Particles The Atmospheric Turbulence Diffusion Laboratory program (DRY DEPOSITION) used in the MGCP, calculates the deposition velocities of sulfur dioxide, ozone, nitric acid vapor, and sulfate particles from meteorological and site specific biological information. Site information includes: major and minor ------- Table 1. Concurrent Growing Season Wet Deposition Via Precipitation kg ion/ha/mo Location Greenville, ME(Howland) Whiteface, NY Hubbard Brook, NY (Moosilauke) Whitetop, VA Clingmans Peak (Mt. Mitchell, NC) Big Meadows, VA (Shenandoah) NH4 + 0.11 0.33 1.11 0.28 0.11 0.31 0.14 0.46 0.12 0.48 0.92 so42- 1.28 2.27 1.18 2.84 2.16 3.20 2.84 5.15 2.69 2.32 2.90 Table 2. Average Ion Concentrations in 1986-1988 Cloud H + Whiteface-1 171 Whiteface-2 225 Moosilauke 263 Shenandoah 171 Whitetop 1 74 Mt. Mitchell 398 so42- 205 352 257 176 321 489 A/03- 73 92 732 94 144 174 N03" 0.65 0.95 0.93 1.46 1.10 1.32 1.17 2.26 1.19 1.43 1.34 Water (jieg/L) NH4 + 97 157 107 93 152 184 Year Elevation 1987 322 m 1987 622 m 1988 1987 250 m 1988 1987 1689m 1988 1987 1987m 1988 1987 1074 m 1988 Elevation Cloud (m) Frequency* 1483 37% 1245 1000 19% 1015 11% 1689 30% 1950 29% *% of hours in cloud. Table 3. Mean Ion Concentrations for 108 Simultaneously Collected Cloud Water Samples 1987/88 (fj.equiv/L) H + SO42- NO3- W/V Whiteface-1 Whiteface-2 122 218 79 151 48 85 74 142 plant species type, leaf area index for plant species, and site location. All available meteorological data including canopy wetness and rainfall are also used. The growing season dry deposition flux is presented in Table 5 for 1987/88, derived by multiplying weekly deposition velocities (model calculation) by the appropriate weekly averaged concen- trations at each site. As is the case with cloud deposition, the northern sites receive generally less dry deposition than the southern sites due to mainly differences in canopy structure. This is particularly obvious for the Shenandoah site which is the only non-coniferous site within MCCP. With the exception of ozone, all other pollutants showed very low ambient concentrations. Therefore, only doses for ozone are calculated in MCCP and presented in Table 6. In addition to the MCCP sites, other nearby ozone monitoring stations have been included for the characterization of forest exposure. In order to provide a biologically relevant value, the sum of season dose (ppm/hr) is calculated by summing up all ozone values above 70 ppb occurring during daylight hours (7 am - 6 pm) of the growing season. The exposure data (dose) in Table 6 suggests a significant north-south gradient and an elevational gradient within a region. The data also show a pronounced year to year change in ozone dose for most of the stations with the 1988 exposure higher by about a factor of two. Howland, the most northeasterly site received the lowest ozone dose, while the most southern sites, Mt. Mitchell and Whitetop, experienced highest exposure. Summary The average monthly sulfur and acidic nitrogen deposition fluxes determined to date (October 1989) for the MCCP sites and for the 1987-88 growing seasons are summarized in Table 7. From these data it is possible to estimate the importance of cloud deposition to the overall flux of pollutants received by the forest ------- Table 4. Calculated Growing Season Cloud Deposition Flux (kg ion/ha) Moosilauke Whiteface-2' Whitetop A Whitetop B~ Mt. Mitchell 1986 1987 1988 1986 1987 1988 1986 1987 1988 1986 1987 1988 1986 1987 1988 Cloud Water Flux (cm) 12.9 10.1 3.5 11.6 10.5 6.0 53.1 39.4 34.3 77.3 61.2 54.3 33.5 27.5 21.8 so42- 21 15 6 11 10 6 83 64 56 135 108 95 52 51 76 A/03- 76 11 5 3 4 2 41 32 29 65 53 48 25 25 18 NH4 + 3.4 2.4 1.0 1.9 1.7 1.2 14.0 10.8 9.5 22.1 17.7 15.6 6.9 6.9 5.0 "There is no forest on top of Whiteface Summit (WF-1). Therefore, deposition has been calculated on a canopy structure slightly above (WF-2). ~ Higher canopy density than Whitetop A. Table 5. Monthly Mean Growing Season Dry Deposition (kg species/ha/mo) Howland Moosilauke Whiteface Shenandoah Whitetop Mt. Mitchell 1987 1988 1987 1988 1987 1988 1987 1988 1988 1987 1988 S02 0.22 0.28 0.30 0.51 3.06 0.75 0.39 1.48 SO/- HNO3 O3 0.11 0.29 5.48 0.15 0.37 5.39 5.96 0.31 1.61 6.57 0.36 6.46 0.28 6.09 0.80 14.06 14.83 11.95 1.64 7.7 12.7 canopy .Although it must be kept in mind that cloud interception is highly dependent upon canopy structure and location above cloud base, it can be nevertheless concluded, that cloud deposition can deliver to the canopy the same and up to four times the amount of pollutants as precipitation does (see Table 8).At the cloud free Howland site, dry deposition appears to account for less than one third of the total acidic substances deposited. The Shenandoah site has a very low cloud impaction frequency due to its relatively low elevation and dry deposition appears to be of greater relative importance (deciduous trees). The estimates for Whiteface suggest that dry sulfurdeposition accounts for less than a quarter of the total sulfur deposition flux. Based on these research results, it can be concluded that any assessment of forest damage at high elevations must take all delivery mechanisms into account, in particular, cloud deposition. ------- Table 6 Ozone Exposure - Total Season April 15 - October 15 (Daylight Hours 7 AM - 6 PM) Sum of Season Dose (ppm'hr) > 0.07 ppm Site Name/State How/and Forest, ME Moosilauke, NH Whiteface Mountain-1, NY Whiteface Mountain-3, NY Whiteface Mountain-4, NY Huntington, NY Hampshire Co., MA Beaver Co., PA Shenandoah-i , VA Shenandoah-2, VA Shenandoah-3, VA Big Meadow, VA Dickey Ridge, VA Sawmill Run, VA Whitetop, TN Giles Co., TN Marion, VA Mt. Mitchell -1, NC Ml Mitchell-2, NC 1986 ND. N D 2 29 ND N D. 509 9 14 N D. N.D ND. ND. 5 56 3 21 11.39 ND. 1638 411 8.34 ND 1987 0.82 7.81 9.68 9.41 3.47 5.74 9.26 13.06 9.49 9.01 6.07 28.50 31.07 26.80 38.54 16.73 9.27 5.14 6.68 1988 4.16 12.51 20.85 16.5 N.D 11.36 34.93 31.70 23.27 39.44 20.88 31.89 40.25 30.16 37.68 28.91 26.92 45.17 19.49 Elevation (m) 250 1000 1483 1026 604 500 312 1300 1015 716 524 1071 631 453 1689 244 710 1950 1750 Table 7. Estimated 1987-88 Deposition Budgets at MCCP Sites Growing Season Mean Sulfur and Nitrogen Deposition (kg S or N/ha-mo) Wet Cloud Dry Howland Moosilauke White face -2 Shenandoah Whitetop Mt. Mitchell S 0.43 0.84 0.58 0.99 1.01 1.31 N 0.15 0.29 0.21 0.28 0.28 0.39 S N no clouds 0.69 0.35 0.65 0.17 insufficient data 3.58 1.23 2.65 0.87 S 0.17 0.31 1.80 N 0.08 0.23 Table 8. Estimated Cloud-to-Wet Depsition Flux Ratios for 1987-88 Growing Season Sulfate Nitrate Moosilauke Whiteface -2 Whitetop Mt. Mitchell 0.8 1.1 3.5 2.0 1.2 0.8 4.4 2.2 ------- ------- ------- Volker A. Mohnen is with the State University of New York at Albany, Albany, NY 12222. Ralph Baumgardner is the EPA Project Officer (see below). The complete report, entitled "An Assessment of Atmospheric Exposure and Deposition to High Elevation Forests in the Eastern United States," (Order No. PB 91-100 1641 AS; Cost: $31.00 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: Atmospheric Research and Exposure Assessment Laboratory U.S. Environmental Protection Agency Research Triangle Park, NC 27711 United States Center for Environmental Research Environmental Protection Information Agency Cincinnati OH 45268 Official Business Penalty for Private Use $300 EPA/600/S3-90/058 ------- |