Effects of macrophytes and external carbon sources on nitrate removal from groundwater in constructed wetlands

Several microcosm wetlands unplanted and planted with five macrophytes (Phragmites australis, Commelina communis, Penniserum purpureum, Ipomoea aquatica, and Pistia stratiotes) were employed to remove nitrate from groundwater at a concentration of 21-47 mg NO3-N/l. In the absence of external carbon, nitrate removal rates ranged from 0.63 to 1.26 g NO3-N/m2/day for planted wetlands. Planted wetlands exhibited significantly greater nitrate removal than unplanted wetlands (P<0.01), indicating that macrophytes are essential to efficient nitrate removal. Additionally, a wetland planted with Penniserum showed consistently higher nitrate removal than those planted with the other four macrophytes, suggesting that macrophytes present species-specific nitrate removal efficiency possibly depending on their ability to produce carbon for denitrification. Although adding external carbon to the influent improved nitrate removal, a significant fraction of the added carbon was lost via microbial oxidation in the wetlands. Planting a wetland with macrophytes with high productivity may be an economic way for removing nitrate from groundwater. According to the harvest result, 4-11% of nitrogen removed by the planted wetland was due to vegetation uptake, and 89-96% was due to denitrification.     

Reduced nitrogen has a greater effect than oxidised nitrogen on dry heathland vegetation

We investigated the effects of different ratios of reduced (NH4+) versus oxidised (NO3(-)) nitrogen in deposition on heathland and species-rich grassland vegetation at high nitrogen deposition levels in large mesocosms filled with nutrient-poor soils to which different NH4+/NO3(-) ratios were applied. The response of the forbs, Antennaria dioica, Arnica montana, Gentiana pneumonanthe, Thymus serpyllum, the grasses Danthonia decumbens, Deschampsia flexuosa, Nardus stricta and the shrub Calluna vulgaris was recorded. The forb A. dioica and the grass D.decumbens preferred low NH4+/NO3(-) ratios and were characterised by a negative correlation between NH4+/NO3(-) ratios and biomass and survival, whereas the grasses N. stricta and D. flexuosa showed no correlation with NH4+/NO3(-) ratios. Lime addition eliminated the negative effects of high NH4+ concentrations in deposition for A. dioica and the grass D. decumbens. The implications of these findings for heathland vegetations are discussed.     

Nitrogen biogeochemistry in the Adirondack Mountains of New York: hardwood ecosystems and associated surface waters

Studies on the nitrogen (N) biogeochemistry in Adirondack northern hardwood ecosystems were summarized. Specific focus was placed on results at the Huntington Forest (HFS), Pancake-Hall Creek (PHC), Woods Lake (WL), Ampersand (AMO), Catlin Lake (CLO) and Hennessy Mountain (HM). Nitrogen deposition generally decreased from west to east in the Adirondacks, and there have been no marked temporal changes in N deposition from 1978 through 1998. Second-growth western sites (WL, PHC) had higher soil solution NO(3-) concentrations and fluxes than the HFS site in the central Adirondacks. Of the two old-growth sites (AMO and CLO), AMO had substantially higher NO(3-) concentrations due to the relative dominance of sugar maple that produced litter with high N mineralization and nitrification rates. The importance of vegetation in affecting N losses was also shown for N-fixing alders in wetlands. The Adirondack Manipulation and Modeling Project (AMMP) included separate experimental N additions of (NH4)2SO4 at WL, PHC and HFS and HNO3 at WL and HFS. Patterns of N loss varied with site and form of N addition and most of the N input was retained. For 16 lake/watersheds no consistent changes in NO(3-) concentrations were found from 1982 to 1997. Simulations suggested that marked NO(3-) loss will only be manifested over extended periods. Studies at the Arbutus Watershed provided information on the role of biogeochemical and hydrological factors in affecting the spatial and temporal patterns of NO(3-) concentrations. The heterogeneous topography in the Adirondacks has generated diverse landscape features and patterns of connectivity that are especially important in regulating the temporal and spatial patterns of NO(3-) concentrations in surface waters.     

Woody stem methane emission in mature wetland alder trees

Methane (CH₄) is an important greenhouse gas that is predominantly emitted to the atmosphere from anoxic wetland ecosystems. Understanding the sources and emissions of CH₄ is crucially important for climate change predictions; however, there are significant discrepancies between CH₄ source estimates derived via so-called bottom-up and top-down methods. Here we report CH₄ emission from the stems of mature wetland alder (Alnus glutinosa) trees in the UK, a common tree of northern hemisphere floodplains and wetlands. The alder stems most likely behave as conduits for soil-produced CH₄ either in the gaseous or aqueous phase, and may, therefore, help to reconcile methodological differences in the way the wetland CH₄ source is estimated.Alder tree stems emitted average peak CH₄ fluxes of 101 μg CH₄ m^?2 h^?1 (on a stem area basis) in early October, a rate that is similar to that obtained from mature Japanese ash (Fraxinus mandshurica var. japonica) in Japan and amounting to approximately 20% of the measured CH₄ flux from the soil surface. The finding suggests that trees, which occupy 60% of Earth's wetlands and are normally excluded from the measurement programmes that form the basis for bottom-up estimates of the global wetland source, could be important contributors to overall terrestrial ecosystem CH₄ flux.     

Responses to ammonium and nitrate additions by boreal plants and their natural enemies

Separate effects of ammonium (NH4+) and nitrate (NO3-) on boreal forest understorey vegetation were investigated in an experiment where 12.5 and 50.0 kg nitrogen (N) ha(-1) year(-1) was added to 2 m2 sized plots during 4 years. The dwarf-shrubs dominating the plant community, Vaccinium myrtillus and V. vitis-idaea, took up little of the added N independent of the chemical form, and their growth did not respond to the N treatments. The grass Deschampsia flexuosa increased from the N additions and most so in response to NO3-. Bryophytes took up predominately NH4+ and there was a negative correlation between moss N concentration and abundance. Plant pathogenic fungi increased from the N additions, but showed no differences in response to the two N forms. Because the relative contribution of NH4+ and NO3- to the total N deposition on a regional scale can vary substantially, the N load a habitat can sustain without substantial changes in the biota should be set considering specific vegetation responses to the predominant N form in deposition.     

Environmental behavior of explosives in groundwater from the Milan Army Ammunition Plant in aquatic and wetland plant treatments. Removal, mass balances and fate in groundwater of TNT and RDX.

Phytoremediation of 2,4,6-trinitrotoluene (TNT) and hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) in groundwater using constructed wetlands is a potentially economical remediation alternative. To evaluate Explosives removal and fate was evaluated using hydroponic batch incubations of plant and substrate treatments with explosives-contaminated groundwater amended with [U-14C]-TNT or [U-14C]-RDX. Plants and substrates were collected from a small-scale wetland constructed for explosives removal, and groundwater originated from a local aquifer at the Milan Army Ammunition Plant. The study surveyed three aquatic, four wetland plant species and two substrates in independent incubations of 7 days with TNT and 13 days with RDX. Parent compounds and transformation products were followed using 14C and chemical (HPLC) analyses. Mass balance of water, plants, substrates and air was determined. It was demonstrated that TNT disappeared completely from groundwater incubated with plants, although growth of most plants except parrot-feather was low in groundwater amended to contain 1.6 to 3.4 mg TNT L-1. Highest specific removal rates were found in submersed plants in water star-grass and in all emergent plants except wool-grass. TNT declined less with substrates, and least in controls without plants. Radiolabel was present in all plants after incubation. Mineralization to 14CO2 was very low, and evolution into 14C-volatile organics negligible. RDX disappeared less rapidly than TNT from groundwater. Growth of submersed plants was normal, but that of emergent plants reduced in groundwater amended to contain 1.5 mg RDX L-1. Highest specific RDX removal rates were found in submersed plants in elodea, and in emergent plants in reed canary grass. RDX failed to disappear with substrates. Mineralization to 14CO2 was low, but relatively higher than in the TNT experiment. Evolution into 14C-volatile organics was negligible. Important considerations for using certain aquatic and wetland plants in constructed wetlands aimed at removing explosives from water are: (1) plant persistence at the explosives level to which it is exposed, (2) specific plant-mass based explosives removal rates, (3) plant productivity, and (4) fate of parent compounds and transformation products in water, plants, and sediments.     

Fate of high loads of ammonia in a pond and wetland downstream from a hazardous waste disposal site

Halls Brook (eastern Massachusetts, USA) is a significant source of total dissolved ammonia (sum of NH(3) and NH(4)(+); (NH(3))(T)) to the Aberjona River, a water body listed for NH(3) impairment on the Clean Water Act section 303(d) list. We hypothesized (1) that (NH(3))(T) in Halls Brook derived from a hazardous waste site via groundwater discharging to a two-basin pond that feeds the brook; and (2) that transport of (NH(3))(T) to the Aberjona River was controlled by lacustrine and wetland processes. To test these hypotheses we measured (NH(3))(T) levels in the brook, the pond, and a wetlands directly downstream of the pond during both dry and wet weather over a ten month period. In addition, we analyzed sediment cores and nitrogen isotopes, and performed mass balance calculations. Groundwater discharge from beneath the hazardous waste site was the major source of (NH(3))(T) (20-67 kg d(-1)) and salinity to the north basin of the pond. The salty bottom waters of the north basin were anoxic on all sampling dates, and exhibited relatively stable (NH(3))(T) concentrations between 200 and 600 mg Nl(-1). These levels were >100-times higher than typical background levels, and 8-24-times above the acute effects level for (NH(3))(T) toxicity. Bottom waters from the north basin continuously spill over into the south basin contributing approximately 50% of the (NH(3))(T) load entering this basin. The remainder comes from Halls Brook, which receives (NH(3))(T) loadings from as yet unknown sources upstream. During storm events up to 50% of the mass of (NH(3))(T) was flushed from the south basin and into the wetlands. The wetlands acted as a (NH(3))(T) sink in dry weather in the growing season and a discharge-dependent (NH(3))(T) source to the Aberjona River during rainstorms.     

复合型人工湿地脱氮效能及其水力负荷影响规律

复合型人工湿地越来越多地被应用在面源污染管理中。不同类型的人工湿地对氮素的去除机理和去除性能是不同的。氮素在湿地生态系统中的去除受多种因素的影响和制约,不同的研究中氮素的去除效率变化较大。通过对韩国西部一复合型人工湿地中氮素的去除能力研究,分析了氮素的去除效率以及水力负荷对去除性能的影响,进而分析了人工湿地去除氮素的主要机理。结果表明,氨氮（NH＋4-N）、硝酸盐氮（NO-3-N）、凯式氮（TKN）和总氮（TN）的平均去除效率分别为13%、29%、35.3和26%。其中有机氮的去除是该复合型人工湿地中氮素去除的主要原因。水力负荷和先行干期天数对氮素的去除能力有一定影响。较长的先行干期天数和较低水力负荷可以提高氮素的去除效率。     

Heavy metal accumulation in trees growing on contaminated sites in Central Europe

Metal-accumulating woody species have been considered for phytoextraction of metal-contaminated sites. We investigated Zn and Cd accumulation in tissues of adult trees and associated herbaceous species collected from contaminated areas in Central Europe. We found considerable Cd and Zn accumulation in various willow, poplar and birch species with up to 116mgCdkg(-1) and 4680mgZnkg(-1) in leaves of Salix caprea. Annual variation of Cd and Zn concentrations in leaves of Salix caprea were small, indicating that data obtained in different years can be compared. Metal concentrations in leaves were not related to total (aqua regia) or labile (1M NH(4)NO(3) extract) concentrations in soil but the accumulation factors (leaf concentration: soil concentration) for Cd and Zn followed an inverse log type function. Metal partitioning between tissues showed a minimum in the wood, with increasing concentrations of Cd and Zn towards the leaves and fine roots.     

不同C／N下人工湿地的脱氮效果及其强化措施

以人工湿地为研究对象,分析了不同C／N下人工湿地的脱氮效果。结果表明,C／N为10时,TN、NO2-N和COD平均去除率分别为（75．36±10．55）％、（86．34±9．23）％和（67．60±4．10）％,都显著高于其他2组系统（P=0．006、0．001、0〈0．01）;随着C／N的增加,NO3-N去除率呈现出上升的趋势;NH4-N刚好相反,C／N为1时,明显要高于其他2种情况（P=0〈0．05）,平均去除率为（65．42-1-14．31）％。针对C／N为1时人工湿地脱氮效率较低（51．294-14．48）％的情况,对系统进水采取了添加一定量好氧反硝化细菌固定化小球并曝气12h的强化实验措施。结果发现,强化实验条件下TN、NOr-N和N03-N去除率均提高了10％以上,且都要明显高于非强化实验条件（P：0．003、0、0〈0．01）,同时NH4-N和COD去除率没有明显差异,研究结果表明,从微生物角度对系统进水进行前处理有助于提高人工湿地脱氮效率。     

Removal efficiency of a constructed wetland for wastewater treatment according to vegetation dominance

A free water surface wetland was built to treat wastewater containing metals (Cr, Ni and Zn) and nutrients from a tool factory in Santo Tomé, Santa Fe, Argentina. Eichhornia crassipes became dominant and covered about 80% of the surface throughout the first year, and decreased progressively until its disappearance. When water depth was lowered Typha domingensis steadily increased plant cover and attained 30% of the surface by the end of the study. While E. crassipes was dominant, the wetland retained 62% of the incoming Cr and 48% of the Ni. NO3- and NO2-, were also removed (65% and 78%, respectively), while dissolved inorganic phosphate (i-P(diss)) and NH4+ were not removed. Zn was below 50 microg l(-1) in both the influent and effluent. Metal concentration in the sediments did not increase and retention was mediated through macrophytes uptake. During the period of E. crassipes decline the wetland retained 49% of the incoming Cr, 45% of Ni, 58% NO3-, 94% NO2-, 58% NH4+ and 47% i-P(diss). Cr, Ni and Zn in the bottom sediment increased in the inlet but not in the outlet. Since T. domingensis became dominant, retention was 58% Cr, 48% Ni and 64% i-P(diss), while 79% NO3-, 84% NO2- and 13% NH4+ were removed. Metals in the bottom sediment increased in the inlet. In spite of the significant growth of E. crassipes at the beginning, T. domingensis remained after most of the transplanted macrophytes had disappeared. Macrophyte disappearance could be related to the overall toxicity of several environmental constrains as high pH and conductivity, metal concentration, and sulphide presence.     

Spatial variability of ammonium and nitrate in soils near a poultry farm

This paper assesses the distribution of ammonium (NH4+) and nitrate (NO3-) nitrogen deposition in native bushland soil adjacent to an open ventilated poultry farm. The farm is located in Thirlmere 150 km south west of Sydney, Australia. A total of 104 geographically referenced soil cores were obtained from the study area. Soil pH, electrical conductivity (EC), NH4(+) - and NO3(-)-nitrogen concentrations were analysed for variable trends at three depths, i.e. 0-30, 30-60, and 60-90 cm. Significantly higher concentrations of the two nitrogen forms and EC were observed nearer to the farm in the surface soil samples (0-30 cm). The distribution of NH4+, NO3- and EC were all correlated in surface samples throughout the study area. There was no indication of NH4+ and NO3- leaching within soil profile sampled and it appears that weeds and native vegetation had utilised the accumulated nitrogen. The level of N deposition adjacent to the poultry farm decreased downwind due to dispersion of plume and to the buffering effects from the bushland.     

Throughfall chemistry in a spruce chronosequence in southern Poland

The chemical composition of throughfall and canopy leaching, as well as the acid neutralizing capacity and alkalinity depended on the age of Norway spruce (Picea abies Karst) stands and season of the year. A higher amount of sulphur and strong acids was deposited to the soil in the older age classes. Concentrations of SO(4)(2)(-), K(+), H(+), Mn(2+), Fe(2+) and Zn(2+) in throughfall were higher than in bulk precipitation in any season. This suggests that these ions were washed out or washed from the surface of needles and/or barks. The other ions NO(3)(-), NH(4)(+), Ca(2+) and Mg(2+) were retained by the canopy, in particular Ca(2+) and Mg(2+) during the growing season in young stands. Principal component analysis identified five factors responsible for the data structure and suggested the major anthropogenic emission sources were acidic emission (SO(4)(2)(-)+NO(3)(-)), heavy metals-dust particles (Fe(2+)+Mn(2+)+Zn(2+)), ammonium (NH(4)(+)) and H(+), while the natural-origin emission was mineral dust (Na(+)+K(+)+Ca(2+)+Mg(2+)).     

Nitrogen deposition in California forests: a review

Atmospheric concentrations and deposition of the major nitrogenous (N) compounds and their biological effects in California forests are reviewed. Climatic characteristics of California are summarized in light of their effects on pollutant accumulation and transport. Over large areas of the state dry deposition is of greater magnitude than wet deposition due to the arid climate. However, fog deposition can also be significant in areas where seasonal fogs and N pollution sources coincide. The dominance of dry deposition is magnified in airsheds with frequent temperature inversions such as occur in the Los Angeles Air Basin. Most of the deposition in such areas occurs in summer as a result of surface deposition of nitric acid vapor (HNO3) as well as particulate nitrate (NO3-) and ammonium (NH4+). Internal uptake of gaseous N pollutants such as nitrogen dioxide (NO2), nitric oxide (NO), HNO3, peroxyacetyl nitrate (PAN), ammonia (NH3), and others provides additional N to forests. However, summer drought and subsequent lower stomatal conductance of plants tend to limit plant utilization of gaseous N. Nitrogen deposition is much greater than S deposition in California. In locations close to photochemical smog source areas, concentrations of oxidized forms of N (NO2, HNO3, PAN) dominate, while in areas near agricultural activities the importance of reduced N forms (NH3, NH4+) significantly increases. Little data from California forests are available for most of the gaseous N pollutants. Total inorganic N deposition in the most highly-exposed forests in the Los Angeles Air Basin may be as high as 25-45 kg ha(-1) year(-1). Nitrogen deposition in these highly-exposed areas has led to N saturation of chaparral and mixed conifer stands. In N saturated forests high concentrations of NO3- are found in streamwater, soil solution, and in foliage. Nitric oxide emissions from soil and foliar N:P ratios are also high in N saturated sites. Further research is needed to determine the ecological effects of chronic N deposition, and to develop appropriate management options for protecting water quality and managing plant nutrient resources in ecosystems which no longer retain excess N.     

Bulk deposition in a rural area located around a large coal-fired power station, northeast Spain

This work focuses on bulk deposition in a rural area located around a large coal-fired power station in northeast Spain. Deposition chemistry was characterised by high concentrations of SO(4)(2-), Ca(2+) and NH(4)(+), which were relatively high when compared with other rural areas. Monthly bulk deposition evolution of major ions was the result of two superimposed patterns: one pattern related to the volume of precipitation and the other showed the seasonal influence of the major ionic sources. A major local origin was attributed to bulk deposition of SO(4)(2-), NH(4)(+), and Ca(2+), whereas a relatively higher contribution of an external source was deduced for NO(3)(-), Na(+) and Cl(-). The SO(4)(2-) concentrations showed a significant correlation with the local SO(2) emissions. High levels of Ca(2+) were due to the high alkalinity of soils in the study area, although an external origin was attributed to the frequent air mass intrusions from the Sahara. Sources of NH(4)(+) were related to intensive livestock farming in the area. Total suspended particles exert a marked influence over bulk deposition and neutralisation. Thus, despite the high emissions of SO(2) in the area, neutral pH values have always been attained given that the concentrations of Ca(2+) and NH(4)(+) account for the total neutralisation of NO(3)(-) and SO(4)(2-).     

高速泳动床对村镇微污染水体的预处理效果

利用高速泳动床反应器作为预处理装置处理村镇微污染水体,出水进入组合人工湿地。结果表明,实验阶段高速泳动床在HRT为1.2 h时,尽管泳动床进水各污染物浓度较低,但反应器对COD、TN和TP仍具有较明显（P〈0.05）的去除效果,平均去除率分别为11.3%、14.6%和25.8%。高速泳动床反应器对氨氮去除效果尤为明显,去除率达到46.9%。此外,高速泳动床反应器内硝化作用较强,出水中硝态氮含量平均增加率为45.5%,弥补了后续人工湿地硝化作用不强、除氨氮效果不佳的缺点。     

Atmospheric input of elements to forest ecosystems: a method of estimation using artificial foliage placed above rain collectors

Usefulness of a method of artificial foliage was tested for estimation of total ionic inputs from the atmosphere to forest ecosystems, as well as of processes relevant to ionic fluxes through tree canopies: uptake, leaching, passive flow. The studies were performed in Norway spruce and European beech stands in Karkonosze Mountains (Poland), in 1995-97. Artificial leaves of increasing leaf area index: 0, 2, 6 and 12 m(2) m(-2 )were placed above standard rain collectors. It has been found that total atmospheric fluxes of H(+), NH(4)(+), Ca(2+), Mg(2+), Pb(2+), NO(3)(-) and SO(4)(2-) rose as surface area of the foliage increased. This was especially true for nitrate, sulphate and ammonium. No such relationship was found for K(+), Na(+), Zn(2+), Cd(2+), Cu(2+) and PO(4)(3-). The increase in anion fluxes exceeded that in neutralising cations (NH(4)(+), Na(+), K(+), Mg(2+), Ca(2+)) and led to progressive rainwater acidification with the increase in the foliage area. An analysis of net canopy exchange (atmospheric input-throughfall flux) has shown that SO(4)(2-), PO(4)(3-), Na(+), Ca(2+) and Cu(2+) flowed passively through the tree crowns; NH(4)(+), NO(3)(-), Zn(2+), Cd(2+) and occasionally Pb(2+) were efficiently absorbed, whereas K(+) was leached from the canopies. Beech was more effective in modifying ionic pool from the atmosphere than spruce. This related to H(+) (greater absorption) and Mg(2+) (greater leaching). It has been demonstrated that the results concerning trends in net canopy exchange and produced by the simple method of artificial foliage are comparable to more sophisticated techniques of the measurements. This proves the method to be useful.     

复合人工湿地对高污染性河流营养物的去除

为了研究复合人工湿地对高污染性河流营养物的去除效果,在西安皂河人渭处建立了一座占地约13334m。包括5组不同复合人工湿地工艺的中试系统。经过1年的实验研究表明,复合型人工湿地对COD、BOD。和ss有很好的去除效果,其去除率最高分别为（82．4±7．2）％、（97．1±1．7）％和（94±2．7）％,对于脱氮除磷而言,以水力停留时间4．1d的复合湿地系列4的处理效果最佳,对TN、NH3-N和TP的年去除率达（79．4±14）％、（79．2±13．7）％和（82．3±12）％。氮的去除效果受温度季节性变化影响较大,夏季平均水温高于19℃有更好的处理效果,磷的去除效果受温度影响不大;NO2-、NO3-去除率呈现负增长,在湿地尾端出现了不同程度的积累。     

The potential use of constructed wetlands in a recirculating aquaculture system for shrimp culture

A pilot-scale constructed wetland unit, consisting of free water surface (FWS) and subsurface flow (SF) constructed wetlands arranged in series, was integrated into an outdoor recirculating aquaculture system (RAS) for culturing Pacific white shrimp (Litopenaeus vannamei). This study evaluated the performance of the wetland unit in treating the recirculating wastewater and examined the effect of improvement in water quality of the culture tank on the growth and survival of shrimp postlarvae. During an 80-day culture period, the wetland unit operated at a mean hydraulic loading rate of 0.3 m/day and effectively reduced the influent concentrations of 5-day biochemical oxygen demand (BOD5, 24%), suspended solids (SS, 71%), chlorophyll a (chl-a, 88%), total ammonium (TAN, 57%), nitrite nitrogen (NO2-N, 90%) and nitrate nitrogen (NO3-N, 68%). Phosphate (PO4-P) reduction was the least efficient (5.4%). The concentrations of SS, Chl-a, turbidity and NO3-N in the culture tank water in RAS were significantly (P相似文献   

Effects of changes in sulfate,ammonia, and nitric acid on particulate nitrate concentrations in the southeastern United States

A thermodynamic equilibrium model, Simulating Composition of Atmospheric Particles at Equilibrium (SCAPE2), was used to investigate the response of fine particulate NO3(-) to changes in concentrations of HNO3, NH3, and SO4(2-) in the southeastern United States. The data consisted of daily, 24-hr time resolution measurements from the Aerosol Research Inhalation Epidemiology Study (ARIES) Jefferson Street (Atlanta) site and five other sites of the Southeastern Aerosol Research and Characterization Project (SEARCH). Reductions of total NH3 (gas-phase NH3 plus particulate NH4(+)), total NO3(-) (HNO3 plus particulate NO3(-)), SO4(2-), or combined total NO3(-) (HNO3 plus particulate NO3(-)) with SO4(2-) were used to estimate the effects of changing emission levels. The conversion of SO2 to SO4(2-) and NO2 to HNO3 involves additional nonlinear reactions not incorporated into the model. For all sites, fine particulate NO3(-) concentrations decreased in response to reductions of either NH3 or total NO3(-), but the particulate NO3(-) decreases were greater for the NH3 reductions than for the total NO3(-) reductions. Particulate NO3(-) concentrations increased in response to reductions of SO4(2-). For the combined reduction (total NO3(-) plus SO4(2-)), the resulting particulate NO3(-) concentrations were on average no different than the base-case NO3(-) levels. Measurements of fine particulate NO3(-) and HNO3 support the modeling conclusions and indicate that particulate NO3(-) formation is limited by the availability of NH3 at most times at all SEARCH sites.