Atmospheric deposition of sulphur and nitrogen species in the U.K.

1. The foundations of our understanding of acid deposition were laid in the last century, but the scale and scope of damage to sensitive receptors has only been subject to intensive investigation over the last 30 years or so. Negotiations are now well underway to reduce emissions, and for some pollutants policy is in place, so that these receptors may be protected adequately. Crucial to this has been the 'critical loads' approach adopted in the U.K. and elsewhere in Europe over the last 6 years.
2. This paper describes the source of acidic emissions, how these emissions are transformed in the atmosphere and subsequently deposited. Measurements of wet deposition are made at a number of sites in the U.K. and some of the results from the networks are presented. These results allow wet and dry deposition to be mapped and the methodologies and underlying assumptions to these procedures are described, and S deposition has been estimated for the U.K. Acid Waters Monitoring Network sites.     

Class I areas at risk: event-based nitrogen deposition to a high-elevation,western site

Between June 1, 2000 and September 30, 2000, 32 precipitation events were sampled near Telluride, CO at an elevation of 3200 m. The wet deposition site was operated following protocols of the Atmospheric Integrated Research Monitoring Network (AIRMoN), a network of the National Atmospheric Deposition Network (NADP). Inorganic nitrogen deposition at the Telluride site of 1.41 kg ha(-1) during the study period was 25 to 50% higher than nearby NADP sites. In turn, nitrogen deposition at these NADP sites was similar to high-elevation sites in and near the Colorado Front Range that have been shown to be impacted by atmospheric deposition of inorganic nitrogen in wetfall. Power plant emissions are a likely source of a major portion of this elevated inorganic nitrogen in wetfall to the San Juan Mountains. Principal component analysis (PCA) shows that solutes formed by gases that are emitted from power plants were clustered tightly together, including nitrate, ammonium, sulfate, and chloride. Trajectory analysis, including both backward and forward trajectories, shows that the air masses that contributed to the precipitation events with high amounts of nitrogen deposition at the Telluride site passed directly over or near power plants. Our results suggest that Class I Wilderness Areas in and near the San Juan Mountains are at risk to ecosystem impairment at present rates of atmospheric deposition of inorganic nitrogen in wetfall. Deployment of proposed power plants to this area will likely increase the risk of degradation of resource values in nearby Class I areas. While these data were collected over a short time span, they indicate that establishment of an official AIRMoN site in the southwestern U.S. may be warranted.     

Monitoring acid waters in the U.K.: an overview of the U.K. Acid Waters Monitoring Network and summary of the first interpretative exercise

1. The U.K. Acid Waters Monitoring Network (AWMN) was established in 1988. It comprises eleven lake and eleven stream sites located throughout the U.K. in areas sensitive to acidification. The principal objective of the AWMN is to provide a long-term, high-quality chemical, biological and palaeolimnological record which, in conjunction with the U.K. precipitation monitoring networks, will facilitate the assessment of trends within U.K. surface waters.
2. The first interpretation of results generated by the AWMN (April 1988–March 1993) has recently been completed and is summarized. During this period there have been no sustained changes in atmospheric deposition in the U.K. Trends are recognized in certain chemical and/or biological parameters at individual AWMN sites, but despite some (regional) patterns no regional trends toward increasing or decreasing acidification are apparent. The data comprise an excellent baseline with which future changes may be compared.
3. The methodology of the AWMN is reviewed and some amendments are suggested in the light of the first 5 years experience. These include: additional determinations for nitrogen species and total phosphorus; changes to the frequency of macrophyte and palaeolimnological sampling; new emphasis on data generated by sediment traps at lake sites; and the addition of extra sites to address better the full extent of acid-sensitive surface waters revealed by the national critical loads mapping programme, and to pay particular attention to the acidifying role of nitrogen.
4. The contribution of AWMN data to other national and international environmental monitoring programmes is highlighted. In addition, AWMN sites provide data to develop and validate critical loads models and dynamic models of acidification, and could also be used to monitor the impact of other air pollutants such as trace metals and persistent organic compounds on the freshwater environment.     

Monitoring acid waters in the U.K.: an overview of the U.K. Acid Waters Monitoring Network and summary of the first interpretative exercise

1. The U.K. Acid Waters Monitoring Network (AWMN) was established in 1988. It comprises eleven lake and eleven stream sites located throughout the U.K. in areas sensitive to acidification. The principal objective of the AWMN is to provide a long-term, high-quality chemical, biological and palaeolimnological record which, in conjunction with the U.K. precipitation monitoring networks, will facilitate the assessment of trends within U.K. surface waters.
2. The first interpretation of results generated by the AWMN (April 1988–March 1993) has recently been completed and is summarized. During this period there have been no sustained changes in atmospheric deposition in the U.K. Trends are recognized in certain chemical and/or biological parameters at individual AWMN sites, but despite some (regional) patterns no regional trends toward increasing or decreasing acidification are apparent. The data comprise an excellent baseline with which future changes may be compared.
3. The methodology of the AWMN is reviewed and some amendments are suggested in the light of the first 5 years experience. These include: additional determinations for nitrogen species and total phosphorus; changes to the frequency of macrophyte and palaeolimnological sampling; new emphasis on data generated by sediment traps at lake sites; and the addition of extra sites to address better the full extent of acid-sensitive surface waters revealed by the national critical loads mapping programme, and to pay particular attention to the acidifying role of nitrogen.
4. The contribution of AWMN data to other national and international environmental monitoring programmes is highlighted. In addition, AWMN sites provide data to develop and validate critical loads models and dynamic models of acidification, and could also be used to monitor the impact of other air pollutants such as trace metals and persistent organic compounds on the freshwater environment.     

Palaeolimnological evidence for recent chemical and biological changes in U.K. Acid Waters Monitoring Network sites

1. Palaeolimnological evidence is presented for the long-term (post-1850) and recent (post-1970) trends in acidity of eleven sites in the U.K. Acid Waters Monitoring Network.
2. Sites are located throughout the U.K. in areas sensitive to acidification, and results show that all have been acidified since pre-industrial times. Although there is considerable variation in the timing and magnitude of these changes the results are consistent with other evidence of the widespread and severe acidification of sensitive U.K. freshwaters as a result of acidic deposition.
3. The most severely acidified sites generally have the highest critical load exceedance, although there is a only a poor relationship between exceedance and post-1850 pH change ( r = 0.58, P = 0.06) or diatom floristic change ( r = 0.52, P = 0.1). These results highlight the difficulty of inferring biological change or 'damage' in freshwater ecosystems from current national maps of critical load exceedances.
4. Evidence of chemical and biological response to the post-1970 reduction in U.K. S emissions is variable: seven lakes show continued acidification in the 1970s and early 1980s while four appear to have been in steady state. One afforested site shows continued acidification until at least 1990, the year of coring, suggesting that at this site increased scavenging of acid anions following canopy closure and/or increased nitrate leaching have offset the benefits of reduced S deposition.
5. Five sites appear to have been in steady state since the early to mid-1980s, and two show unambiguous evidence for a recent increase in pH and a reversal in the diatom assemblages to that of earlier levels. The results support and extend the findings of other studies and show that biological recovery is occurring in at least two chronically acidified areas of the U.K. (Galloway, SW Scotland, and north Wales), and that natural recovery can lead to the re-establishment of biota previously present at the site.     

Palaeolimnological evidence for recent chemical and biological changes in U.K. Acid Waters Monitoring Network sites

1. Palaeolimnological evidence is presented for the long-term (post-1850) and recent (post-1970) trends in acidity of eleven sites in the U.K. Acid Waters Monitoring Network.
2. Sites are located throughout the U.K. in areas sensitive to acidification, and results show that all have been acidified since pre-industrial times. Although there is considerable variation in the timing and magnitude of these changes the results are consistent with other evidence of the widespread and severe acidification of sensitive U.K. freshwaters as a result of acidic deposition.
3. The most severely acidified sites generally have the highest critical load exceedance, although there is a only a poor relationship between exceedance and post-1850 pH change ( r = 0.58, P = 0.06) or diatom floristic change ( r = 0.52, P = 0.1). These results highlight the difficulty of inferring biological change or 'damage' in freshwater ecosystems from current national maps of critical load exceedances.
4. Evidence of chemical and biological response to the post-1970 reduction in U.K. S emissions is variable: seven lakes show continued acidification in the 1970s and early 1980s while four appear to have been in steady state. One afforested site shows continued acidification until at least 1990, the year of coring, suggesting that at this site increased scavenging of acid anions following canopy closure and/or increased nitrate leaching have offset the benefits of reduced S deposition.
5. Five sites appear to have been in steady state since the early to mid-1980s, and two show unambiguous evidence for a recent increase in pH and a reversal in the diatom assemblages to that of earlier levels. The results support and extend the findings of other studies and show that biological recovery is occurring in at least two chronically acidified areas of the U.K. (Galloway, SW Scotland, and north Wales), and that natural recovery can lead to the re-establishment of biota previously present at the site.     

A spatial analysis of atmospheric ammonia and ammonium in the U.K

As measures are implemented internationally to reduce SO2 and NOx emissions, attention is falling on the contribution of NH3 emissions to acidification, nitrogen eutrophication, and aerosol formation. In the U.K., a monitoring network has been established to measure the spatial distribution and long-term trends in atmospheric gaseous NH3 and aerosol NH4+. At the same time, an atmospheric chemistry and transport model, FRAME, has been developed with a focus on reduced nitrogen (NHx). The monitoring data are important to evaluate the model, while the model is essential for a more detailed spatial assessment. The national network is established with over 80 sampling locations. Measurements of NH3 and NH4+ (at up to 50 sites) have been made using a new low-cost denuder-filterpack system. Additionally, improved passive sampling methods for NH3 have been applied to explore local variability. The measurements confirm the high spatial variability of NH3 (annual means 0.06 to 11 microg NH3 m(-3)), consistent with its nature as a primary pollutant emitted from ground-level sources, while NH4+, being a slowly formed secondary product, shows much less spatial variability (0.14 to 2.4 mg NH4+ m(-3)). These features are reproduced in the FRAME model, which provides estimates at a 5-km level. Analysis of the underlying NH3 emission inventory shows that sheep emissions may have been underestimated and nonagricultural sources overestimated relative to emissions from cattle. The combination of model and measurements is applied to estimate spatial patterns of dry deposition to different vegetation types. The combined approach provides the basis to assess NHx responses across the U.K. to international emission controls.     

The U.K. Acid Waters Monitoring Network: an assessment of chemistry data, 1988–93

1. The current extent and distribution of acidified surface waters in the U.K. is assessed using data collected between 1988 and 1993 as part of the U.K. Acid Waters Monitoring Network (AWMN). The data have been collected against a background of constant S deposition across the U.K. throughout the monitoring period. 2. Surface waters with mean pH < 5.0 occur in south-west Scotland, south-east Northern Ireland, the Lake District and south-east England. In addition, sites with mean pH < 5.5 are found in central and north-east Scotland, the Pennines and north Wales. These areas receive, and have historically received, high levels of S deposition and xSO₄ is identified as the main contribution to non-marine acid anion concentrations. 3. Mean total oxidized nitrogen (TON) concentrations are > 10 μeq l^–1 at ten of the twenty-two sites which are found in areas broadly corresponding to areas of high N deposition. The mean contribution of TON to total non-marine acid anion concentration is > 10% at sixteen sites and > 20% at six sites. Most sites, except for those with TON < 10 μeq l^–1 and mainly located in north-west Scotland and Northern Ireland, demonstrate strong seasonality in TON concentrations and during autumn and winter instantaneous contributions of TON to total non-marine acid anions is up to 60%. This confirms the importance of N with respect to surface water acidification and strengthens the case for implementation of controls on future N emissions. 4. The data period is currently too short for rigorous trend analysis given the monthly/quarterly sampling frequency in streams/lakes, respectively. Nevertheless, increased SO₄ and xSO₄ can be observed in the time series at sites in south-west Scotland and north Wales despite constant deposition to these areas. Similar trends are evident in longer-term more frequent data at two sites and may reflect hydrometeorological influences, especially the duration and intensity of hot and dry weather in summer which promotes mineralization of organic S.     

Developing seasonal ammonia emission estimates with an inverse modeling technique

Significant uncertainty exists in magnitude and variability of ammonia (NH3) emissions, which are needed for air quality modeling of aerosols and deposition of nitrogen compounds. Approximately 85% of NH3 emissions are estimated to come from agricultural nonpoint sources. We suspect a strong seasonal pattern in NH 3 emissions; however, current NH3 emission inventories lack intra-annual variability. Annually averaged NH 3 emissions could significantly affect model-predicted concentrations and wet and dry deposition of nitrogen-containing compounds. We apply a Kalman filter inverse modeling technique to deduce monthly NH3 emissions for the eastern U.S. Final products of this research will include monthly emissions estimates from each season. Results for January and June 1990 are currently available and are presented here. The U.S. Environmental Protection Agency (USEPA) Community Multiscale Air Quality (CMAQ) model and ammonium (NH4+) wet concentration data from the National Atmospheric Deposition Program (NADP) network are used. The inverse modeling technique estimates the emission adjustments that provide optimal modeled results with respect to wet NH4+ concentrations, observational data error, and emission uncertainty. Our results suggest that annual average NH 3 emissions estimates should be decreased by 64% for January 1990 and increased by 25% for June 1990. These results illustrate the strong differences that are anticipated for NH3 emissions.     

Contemporary and pre-industrial global reactive nitrogen budgets

Increases and expansion of anthropogenic emissions of both oxidized nitrogen compounds, NO_x, and a reduced nitrogen compound, NH₃, have driven an increase in nitrogen deposition. We estimate global NO_x and NH₃ emissions and use a model of the global troposphere, MOGUNTIA, to examine the pre-industrial and contemporary quantities and spatial patterns of wet and dry NO_y and NH_x deposition. Pre-industrial wet plus dry NO_x and NH_x deposition was greatest for tropical ecosystems, related to soil emissions, biomass burning and lightning emissions. Contemporary NO_y+NH_x wet and dry deposition onto Northern Hemisphere (NH) temperate ecosystems averages more than four times that of preindustrial N deposition and far exceeds contemporary tropical N deposition. All temperate and tropical biomes receive more N via deposition today than pre-industrially. Comparison of contemporary wet deposition model estimates to measurements of wet deposition reveal that modeled and measured wet deposition for both NO ₃ ^– and NH ₄ ⁺ were quite similar over the U.S. Over Western Europe, the model tended to underestimate wet deposition of NO ₃ ^– and NH ₄ ⁺ but bulk deposition measurements were comparable to modeled total deposition. For the U.S. and Western Europe, we also estimated N emission and deposition budgets. In the U.S., estimated emissions exceed interpolated total deposition by 3-6 Tg N, suggesting that substantial N is transported offshore and/or the remote and rural location of the sites may fail to capture the deposition of urban emissions. In Europe, by contrast, interpolated total N deposition balances estimated emissions within the uncertainty of each.Abbreviations EMEP European Monitoring and Evaluation Program - GEIA Global Emissions Inventory Activity - NADP/NTN National Atmospheric Deposition Program/National Trends Network in the US - NH Northern Hemisphere - NH_x=NH₃+NH ₊ ⁴ NO_x=NO+NO₂ NO_y total odd nitrogen=NO_x+HNO₃+HONO+HO₂NO₂+NO₃+radical (NO₃ ^.)+Peroxyacetyl nitrates+N₂O₅+organic nitrates - SH Southern Hemisphere - Gg 10⁹ g - Tg 10¹² g     

Atmospheric heavy metal input to forest soils in rural areas of Denmark

Atmospheric bulk deposition of heavy metals (HM) was measured from 1972/73 to the present time at five to ten forest sites in rural areas of Denmark. From 1979, HM in aerosols were measured at one to four forest sites. On the basis of these long-term continuous measurements, the atmospheric inputs to the forest floor have been calculated. Yearly HM emission estimates to the European atmosphere seems to correlate well with yearly average values of HM deposition, as well as with HM concentrations in the ambient atmosphere. HM emissions have been estimated since the 1950s. Using the correlation between emission and deposition, HM deposition values maybe extrapolated in reverse chronological order. The accumulated atmospheric HM deposition has been estimated in this way over a period of 50 years.     

A case study of nitrogen saturation in western U.S. forests

Virtually complete nitrification of the available ammonium in soil and nitrification activity in the forest floor are important factors predisposing forests in the San Bernardino Mountains of southern California to nitrogen (N) saturation. As a result, inorganic N in the soil solution is dominated by nitrate. High nitrification rates also generate elevated nitric oxide (NO) emissions from soil. High-base cation saturation of these soils means that soil calcium depletion or effects associated with soil acidification are not an immediate risk for forest health as has been postulated for mesic forests in the eastern U.S. Physiological disturbance (e.g., altered carbon [C] cycling, reduced fine root biomass, premature needle abscission) of ozone-sensitive ponderosa pine trees exposed to high N deposition and high ozone levels appear to be the greater threat to forest sustainability. However, N deposition appears to offset the aboveground growth depression effects of ozone exposure. High nitrification activity reported for many western ecosystems suggests that with chronic N inputs these systems are prone to N saturation and hydrologic and gaseous losses of N. High runoff during the winter wet season in California forests under a Mediterranean climate may further predispose these watersheds to high nitrate leachate losses. After 4 years of N fertilization at a severely N saturated site in the San Bernardino Mountains, bole growth unexpectedly increased. Reduced C allocation below- ground at this site, presumably in response to ozone or N or both pollutants, may enhance the bole growth response to added N.     

120 Years of U.S. Residential Housing Stock and Floor Space

Residential buildings are a key driver of energy consumption and also impact transportation and land-use. Energy consumption in the residential sector accounts for one-fifth of total U.S. energy consumption and energy-related CO₂ emissions, with floor space a major driver of building energy demands. In this work a consistent, vintage-disaggregated, annual long-term series of U.S. housing stock and residential floor space for 1891–2010 is presented. An attempt was made to minimize the effects of the incompleteness and inconsistencies present in the national housing survey data. Over the 1891–2010 period, floor space increased almost tenfold, from approximately 24,700 to 235,150 million square feet, corresponding to a doubling of floor space per capita from approximately 400 to 800 square feet. While population increased five times over the period, a 50% decrease in household size contributed towards a tenfold increase in the number of housing units and floor space, while average floor space per unit remains surprisingly constant, as a result of housing retirement dynamics. In the last 30 years, however, these trends appear to be changing, as household size shows signs of leveling off, or even increasing again, while average floor space per unit has been increasing. GDP and total floor space show a remarkably constant growth trend over the period and total residential sector primary energy consumption and floor space show a similar growth trend over the last 60 years, decoupling only within the last decade.     

Josef Rudinger Memorial Lecture 2002. The chemistry of the opioid receptor binding sites.

Since the discovery of the opioid receptors and their endogenous ligands an immense research work has been devoted to the exploration of their specificity, the mechanism of ligand binding and ligand-receptor interactions. One of the main goals has been the location and characterization of the binding sites. The present review compiles the results achieved in this field in the last quarter of a century, and puts some questions concerning the success of these efforts.     

Decreasing nitrogen deposition rates: Good news for oligotrophic grassland species?

Several studies have found that increased nitrogen (N) deposition leads to a decline in species richness in semi-natural grasslands, mainly due to the loss of species typical of nutrient-poor soils. However, after reaching a peak around 1990, N deposition has decreased in Europe over the last 30 years. In this study, we investigated the changes in species number and composition of semi-natural grasslands during this period of declining N deposition. To this end, we compared the data from the first survey (2001-2005) of 147 grassland sites in Switzerland with those from the third survey (2011-2015). We further analysed the vegetation development of a specific hay meadow from 1992 to 2013. In this grassland, total vegetation cover and the cover of graminoid species decreased, while the cover of oligotrophic species increased. At the 147 grassland sites, total species number decreased at sites with still high levels of N deposition and it tended to increase at sites with low N deposition, i. e. below the critical load for N deposition. The number of oligotrophic grassland species increased at sites with a large decrease in N deposition and strong inclination. Thus, the results of this study indicate that the reduction of N emissions had a measurable positive effect on species diversity in these semi-natural grasslands. Most of the grasslands surveyed appear to be quite resilient against N deposition, i. e. they do not shift to an alternative low diversity state dominated by a few competitive species, and recovery of the species composition as a result of the decrease in N deposition seems possible, especially on steep slopes. Furthermore, the study underlines the importance of regular management of semi-natural, unfertilised, low-productivity grassland to maintain the diversity of oligotrophic grassland species.     

Longitudinal evaluation of vegetation richness and cover at wetland compensation sites: implications for regulatory monitoring under the Clean Water Act

There has been regulatory concern over the appropriate length of time to monitor wetland sites restored or created as compensation for impacts permitted by a U.S. Clean Water Act permit. However there is very little longitudinal research on wetland compensation sites, and conclusions on compensation site development are usually drawn from the analysis of a chronosequence of sites of different ages. This approach has limitations, given the extent of changes in wetland compensation practices and performance standards over the past few decades. In this study we conducted vegetation surveys of 22 wetland compensation sites in a rapidly developing part of the Minneapolis-St. Paul metropolitan area in 1997 and 2010. We present data on changes over time in floristic richness and cover at the site level and at the level of wetland community type within each site. Our findings do not support the assumption that wetland compensation sites progress on a trajectory toward increasing diversity, floristic quality, or native cover over time. We find that, when data from all sites are considered together, emergent communities have suffered significant declines in both floristic quality and native plant cover, while wet meadow communities have gained species richness but not species diversity. There is some evidence that site richness and cover characteristics are converging toward a regional mean over time, as the species composition of wet meadows became significantly more similar over the survey period, and all community types have significant increases in woody cover. Our study suggests the importance of selecting appropriate compensation sites that avoid foreseeable hydrologic stresses, and does not support the position that 5 years of monitoring can assure the ongoing biotic integrity of wetland compensation sites.     

The Potential for Carbon Sequestration Through Reforestation of Abandoned Tropical Agricultural and Pasture Lands

Approximately half of the tropical biome is in some stage of recovery from past human disturbance, most of which is in secondary forests growing on abandoned agricultural lands and pastures. Reforestation of these abandoned lands, both natural and managed, has been proposed as a means to help offset increasing carbon emissions to the atmosphere. In this paper we discuss the potential of these forests to serve as sinks for atmospheric carbon dioxide in aboveground biomass and soils. A review of literature data shows that aboveground biomass increases at a rate of 6.2 Mg ha^{? 1} yr^{? 1} during the first 20 years of succession, and at a rate of 2.9 Mg ha^{? 1} yr^{? 1} over the first 80 years of regrowth. During the first 20 years of regrowth, forests in wet life zones have the fastest rate of aboveground carbon accumulation with reforestation, followed by dry and moist forests. Soil carbon accumulated at a rate of 0.41 Mg ha^{? 1} yr^{? 1} over a 100‐year period, and at faster rates during the first 20 years (1.30 Mg carbon ha^{? 1} yr^{? 1} ). Past land use affects the rate of both above‐ and belowground carbon sequestration. Forests growing on abandoned agricultural land accumulate biomass faster than other past land uses, while soil carbon accumulates faster on sites that were cleared but not developed, and on pasture sites. Our results indicate that tropical reforestation has the potential to serve as a carbon offset mechanism both above‐ and belowground for at least 40 to 80 years, and possibly much longer. More research is needed to determine the potential for longer‐term carbon sequestration for mitigation of atmospheric CO₂ emissions.     

丹江口水库淅川库区大气氮湿沉降特征

大气氮沉降是除河流输入外水库水体重要的外源氮输入途径。以丹江口水库淅川库区为研究区,于2018年11月至2019年10月在库区周边设置了6个采样点,采集并分析了库区大气氮湿沉降样品,探讨氮湿沉降的时空分布特征以及对水库水体外源氮输入的贡献。研究结果表明,研究区大气氮湿沉降量为24.21 kg hm^-2 a^-1,其中氨氮占比（47.45％）为最大,有机氮占比（36.34％）次之,硝氮占比（16.21％）最小。硝氮湿沉降量在空间上表现出显著差异性。氨氮、有机氮湿沉降量的季节差异显著,氨氮是以夏季最高,秋季次之,冬季最低,而有机氮是以秋季最高,夏季次之,冬季最低。氨氮、硝氮、有机氮湿沉降量之间存在显著相关性,氨氮、有机氮湿沉降量与降水量之间存在显著相关性。总氮、氨氮湿沉降量分别为1321.98 t/a和627.34 t/a,分别占河流总氮、氨氮入库量的10.82％、34.85％。研究结果可为探索有针对性的库区水体氮污染控制途径提供重要理论基础。     

Trends and variability in weather and atmospheric deposition at UK Environmental Change Network sites (1993–2012)

We characterised temporal trends and variability in key indicators of climate and atmospheric deposition chemistry at the twelve terrestrial UK Environmental Change Network (ECN) sites over the first two decades of ECN monitoring (1993–2012) using various statistical approaches. Mean air temperatures for the monitoring period were approximately 0.7 °C higher than those modelled for 1961–1990, but there was little evidence for significant change in air temperature over either the full monthly records or within individual seasons. Some upland ECN sites, however, warmed significantly over the first decade before cooling in the second. Summers at most sites became progressively wetter, and extremes in daily rainfall increased in magnitude. Average wind speeds in winter and spring declined at the majority of sites. Directional trends in summer precipitation could be linked to an atypically prolonged negative deviation in the summer North Atlantic Oscillation (NAO) Index. Several aspects of air quality improved markedly. Concentrations and fluxes of sulphate in precipitation declined significantly and substantially across the network, particularly during the earlier years and at the most polluted sites in the south and east. Precipitation concentrations of nitrate and ammonium, and atmospheric concentrations of nitrogen dioxide also decreased at most sites. There was less evidence for reductions in the loads of wet deposited nitrogen species, while trends in atmospheric ammonia concentration varied in direction and strength between sites. Reductions in acid deposition are likely to account for widespread gradual increases in the pH of soil water at ECN sites, representing partial recovery from acidification. Overall, therefore, ECN sites have experienced marked changes in atmospheric chemistry and weather regimes over the last two decades that might be expected to have exerted detectable effects on ecosystem structure and function. While the downward trend in acid deposition is unlikely to be reversed, it is too early to conclude whether the trend towards wetter summers simply represents a phase in a multi-decadal cycle, or is indicative of a more directional shift in climate. Conversely, the first two decades of ECN now provide a relatively stable long-term baseline with respect to air temperature, against which effects of anticipated future warming on these ecosystems should be able to be assessed robustly.