Atmospheric Sulfur Deposition Research Articles

Plant functional traits modulate the effects of soil acidification on above- and belowground biomass

Abstract. Atmospheric sulfur (S) deposition has been increasingly recognized as a major driver of soil acidification. However, little is known about how soil acidification influences above- and belowground biomass by altering leaf and root traits. We conducted a 3-year S-addition experiment to simulate soil acidification in a meadow. Grass (Leymus chinensis (Trin.) Tzvelev) and sedge (Carex duriuscula C.A.Mey) species were chosen to evaluate the linkage between plant traits and biomass. Sulfur addition led to soil acidification and nutrient imbalances. Soil acidification decreased specific leaf area (SLA) but increased leaf dry-matter content (LDMC) in L. chinensis, showing a conservative strategy and thus suppressing aboveground instead of belowground biomass. However, in C. duriuscula, soil acidification increased plant height and root nutrients (N, P, S, and Mn), favoring competition for natural resources through enhanced above- and belowground biomass, i.e., adoption of an acquisitive strategy. Increased soil acidity resulted in an overall reduction in aboveground community biomass by 3 %–33 %, but it led to an increase in community root biomass by 11 %–22 % due to upregulation as a result of higher soil nutrient availability. Our results demonstrate that both above- and belowground plant biomass is affected by S-induced acidification. Understanding the linkage between plant biomass and functional traits contributes to a better understanding of plant–soil feedback in grassland ecosystems.

Sulfur Isotope Geochemistry of Ice‐Wedges in Yakutia, East Siberia

ABSTRACTSulfur, with its highly varying stable isotope ratio and involvement in numerous biogeochemical processes, is one of the most widely used elements as an isotopic paleoenvironmental proxy, yet the sulfur isotope ratios of ice‐wedges and their insoluble fraction remain unexplored. This study first presents the sulfur isotopic compositions of soluble sulfate, particulate organic matter (POM), and lithic particles recovered from East Siberian ice‐wedges. Soluble sulfate, primarily representing atmospheric sulfate deposition, shows comparable sulfur isotope ranges in Zyryanka and Batagay, while in Central Yakutia, ice‐wedge sulfate is more enriched in 34S, consistent with the orogenic and cratonic terranes in East Siberia. Given the wedge growth during the inland winter, it is likely that sulfate aerosols were derived mainly from erosion and weathering of regional basement rocks rather than from sea salt spray or biogenic emissions. Within individual ice‐wedges, however, the sulfur isotopic composition of soluble sulfate varies by as much as 7‰, possibly reflecting changes in the relative contributions of sulfur‐isotopically distinct source regions. Beyond the origin of sulfate, greater sulfur isotope fractionations between POM and sulfate during the last glaciation suggest that sulfate may have been anaerobically reduced to sulfide and vice versa in the adjacent root zone.

Climate change could negate U.S. forest ecosystem service benefits gained through reductions in nitrogen and sulfur deposition

Climate change and atmospheric deposition of nitrogen (N) and sulfur (S) impact the health and productivity of forests. Here, we explored the potential impacts of these environmental stressors on ecosystem services provided by future forests in the contiguous U.S. We found that all stand-level services benefitted (+ 2.6 to 8.1%) from reductions in N+S deposition, largely attributable to positive responses to reduced S that offset the net negative effects of lower N levels. Sawtimber responded positively (+ 0.5 to 0.6%) to some climate change, but negatively (− 2.4 to − 3.8%) to the most extreme scenarios. Aboveground carbon (C) sequestration and forest diversity were negatively impacted by all modelled changes in climate. Notably, the most extreme climate scenario eliminated gains in all three services achieved through reduced deposition. As individual tree species responded differently to climate change and atmospheric deposition, associated services unique to each species increased or decreased under future scenarios. Our results suggest that climate change should be considered when evaluating the benefits of N and S air pollution policies on the services provided by U.S. forests.

Do trees respond to pollution? A network study of the impact of pollution on spruce growth from Europe

Tree rings have been reliably used as an environmental proxy over the past decades for environmental reconstructions, simulations and forecasting. In our study, we investigated whether tree-ring chronologies are impacted by pollution. We chose sites in the Krušné hory and the Krkonoše Mountains in the Czech Republic which have a known history of pollution. We sampled Norway spruce (Picea abies [L.] Karst) in both ranges and compared their chronologies. We found no significant difference in the overall radial growth in the chronologies from both regions. However, we observed an increased heterogeneity in the growth of trees from the 1970s till the 1990s. Coherently, a severe reduction in tree growth from the late 1970s and a recovery towards the early 1990s was evident. We collected and analysed soil samples for pH and exchangeable element concentrations. All seven sampling sites' soils were strongly acidic (pHCaCl2 = 3.3 ± 0.4). The average soil base saturation at Krušné hory was higher than at Krkonoše (39% versus 12%), likely due to more intensive liming.Further, we compared these chronologies to other sites in Europe. Analysing 89 sites, we found that most (9 out of 14) of the sites with significantly reduced radial tree growth were located within the former ‘Black Triangle’, an area which was subjected to heavy industrialisation and pollution from the 1960s to the 1990s. Atmospheric sulphur deposition was found to negatively affect radial tree-growth, while limited quantities of oxidised nitrogen appeared to have a positive effect. Our results are consistent with previous research, indicating that atmospheric SO2 pollution and subsequent acid fog and rime have led to a reduction in annual radial tree growth across the Black Triangle.

Geographic variation in projected US forest aboveground carbon responses to climate change and atmospheric deposition

Forest composition and ecosystem services are sensitive to anthropogenic pressures like climate change and atmospheric deposition of nitrogen (N) and sulfur (S). Here we extend recent forest projections for the current cohort of trees in the contiguous US, characterizing potential changes in aboveground tree carbon at the county level in response to varying mean annual temperature, precipitation, and N and S deposition. We found that relative to a scenario with N and S deposition reduction and no climate change, greater climate change led generally to decreasing aboveground carbon (mean −7.5% under RCP4.5, −16% under RCP8.5). Keeping climate constant, reduced N deposition tended to lessen aboveground carbon (mean −7%), whereas reduced S deposition tended to increase aboveground carbon (+3%) by 2100. Through mid-century (2050), deposition was more important for predicting carbon responses except under the extreme climate scenarios (RCP8.5); but, by 2100, climate drivers generally outweighed deposition. While more than 70% of counties showed reductions in aboveground carbon relative to the reference scenario, these were not evenly distributed across the US. Counties in the Northwest and Northern Great Plains, and the northern parts of New England and the Midwest, primarily showed positive responses, while counties in the Southeast showed negative responses. Counties with greater initial biomass showed less negative responses to climate change while those which exhibited the greatest change in composition (>15%) had a 95% chance of losing carbon relative to a no-climate change scenario. This analysis highlights that declines in forest growth and survival due to increases in mean temperature and reductions in atmospheric N deposition are likely to outweigh positive impacts of reduced S deposition and potential increases in precipitation. These effects vary at the regional and county level, however, so forest managers must consider local rather than national dynamics to maximize forest carbon sinks in the future.

Atmospheric deposition of nitrogen and sulphur in the Dniester catchment: the impact of war at a glance

ABSTRACT Burning of fossil fuels, application of fertilisers, and livestock farming have greatly increased emissions of reactive nitrogen (N). The consequent increase in atmospheric deposition of N compounds has compromised air, soil and water quality, ecosystems, and human health and wellbeing. Sulphate aerosols also affect climate dynamics by scattering solar radiation, leading to surface cooling and, indirectly, cloud formation and precipitation. During 2021 (the pre-war year), the rates of total N deposition over the lower, middle and upper parts of the Dniester catchment were 21.8 ± 1.7, 17.0 and 19.0 ± 3.1 kgN/ha, respectively. The war in Ukraine brought a 35% decrease in annual total N deposition within the Lower Dniester region as a consequence of economic disruption and population displacement. In contrast, the influx of refugees and business relocation to the middle and upper parts of the basin counteracted the impacts of war, resulting in a slight increase (ca. 4%) or no change in cumulative total N deposition during 2022 compared to the pre-war year. The pre-war rates of sulphate deposition were 2.8 ± 0.1, 2.8 and 3.2 ± 0.1 kgS/ha for the lower, middle and upper basin: these were reduced 11–15%. These findings emphasise that local and regional factors interact. Peace is a prerequisite for reducing N emissions and safeguarding the environment.

Similarities in Storage and Transport of Sulfate in Forested and Suburban Watersheds, Despite Anthropogenically Elevated Suburban Sulfate

AbstractSulfate is a potential pollutant and important nutrient linked with the nitrogen, carbon, and phosphorus cycles. The importance of different anthropogenic sulfate sources in suburban streams (septic systems, fertilizer, road salt, and infrastructure) is uncertain, and the temporal dynamics of stream export sparsely documented. We study sources and export dynamics of sulfate in suburban and forested headwater catchments. Stream baseflow discharge and sulfate concentrations were strongly positively correlated in both watersheds with the highest values in spring. Suburban concentrations and fluxes (2.48–7.5 mg/L or 25.8–78.1 μM, 16.6 kg/ha/yr) were consistently higher than forested (0.56–2.78 mg/L or 5.8–28.9 μM, 5 kg/ha/yr). Following precipitation, sulfate concentrations in both forested and suburban streams increased to concentrations above pre‐storm values and remained high after peak discharge. These dynamics suggest that both catchments have a large pool of sulfate that can be mobilized under wet conditions. Ridge‐top forest soil samples contained 210 kg/ha stored, extractable sulfate. Current atmospheric sulfate deposition rates (5–7 kg/ha/yr) are approximately in balance with sulfate export in the forested stream. In the suburban watershed, we estimated septic fields contribute up to 11 kg/ha/yr (about half from surfactants) and lawn care up to 4.3 kg/ha/yr and are the most likely sources of elevated stream sulfate. Sulfate sulfur (4.9–5.8‰ forested; 6.1–7.0‰ suburban) and oxygen isotope values (0.7–2.0‰ forested; −0.1–4.1‰ suburban) are consistent with this interpretation, but do not provide strong corroboration due to large variation and overlap in estimated source values.

Atmospheric deposition and soil water chemistry in Swedish forests since 1985 – Effects of reduced emissions of sulphur and nitrogen

Trends for the atmospheric deposition of sulphur (S) and inorganic nitrogen (inorg-N) to forests and changes in the forest soil water chemistry in Sweden have been assessed since 1985, with special focus on the last 25 years, based on measurements within the Swedish Throughfall Monitoring Network (SWETHRO). The reductions in the deposition of S and inorg-N in the southern part of Sweden corresponded relatively well with the pollutant emission reductions for S and inorg-N from both EU27 + UK and Sweden during 1996/97–2021/22. For northern Sweden the deposition of S and inorg-N decreased to a lesser extent than both European and Swedish emissions. The bulk deposition of NO3-N has decreased more than the deposition of NH4-N over the last 25-year period, which is consistent with the much larger emission reductions for NOx compared to NH3 from EU27 + UK and Sweden. The S concentrations in the soil water, at 50 cm below soil surface, have decreased during the last 25 years, however somewhat less than the S deposition. At sites with low ANC and pH in the beginning of the period, the increase in ANC was generally greater and the increase in pH was smaller, but at sites with high pH and ANC above zero, the increase in pH was dominant, in line with the nonlinear relationship between pH and ANC in the soil water. The incidence of elevated concentrations of NO3-N in the soil water was highest in southwest Sweden, ranging between 4 and 19 % of all measuring occasions since 1985/86. The reduced deposition of N over the 35-year period was not reflected in the incidence of elevated concentrations of NO3-N in the soil water over time.

Delayed recovery of surface water chemistry from acidification in subtropical forest region of China

The three largest acid rain regions of current earth are located in northern and western Europe, eastern North America, and East Asia. Sulfur and nitrate concentrations in headwater streams in Europe and North America decreased as atmospheric sulfur and nitrogen deposition decreased, albeit with a considerable delay. However, how water chemistry responds to the declining sulfur and nitrogen deposition in China is unclear. The regional survey of surface water chemistry during 2010 and 2018 within the Sichuan Basin in southwestern China showed that the recovery of the surface water chemistry was delayed for at least 5 years owing to the release of previously deposited sulfur and nitrogen stored in the soil. After sulfur deposition declined from its peak value, the subregions of purplish soil with low sulfate adsorption capacity still exhibited a net sulfur release in 2010, but this release was no longer evident by 2018. The subregions with the red and yellow soils, which have a high sulfate adsorption capacity, operated as sulfur sinks during 2010 and 2018, indicating a continuous immobilization process through sulfate reduction despite a decrease in sulfur deposition. Additionally, this sulfate reduction countered the release of sulfate caused by sulfur desorption. There was a substantial nitrogen sink within the Sichuan Basin. Nitrogen leaching decreased slowly with the declined nitrogen deposition, except in regions where nitrogen deposition exceeded the critical threshold. Compared to temperate forest regions in Europe, the Sichuan Basin and its surrounding areas have experienced higher decline rates in the leaching of sulfur and nitrogen, highlighting that the subtropical forest region undergoes a faster restoration of surface water chemistry.

Future climate change effects on US forest composition may offset benefits of reduced atmospheric deposition of N and S.

Climate change and atmospheric deposition of nitrogen (N) and sulfur (S) are important drivers of forest demography. Here we apply previously derived growth and survival responses for 94 tree species, representing >90% of the contiguous US forest basal area, to project how changes in mean annual temperature, precipitation, and N and S deposition from 20 different future scenarios may affect forest composition to 2100. We find that under the low climate change scenario (RCP 4.5), reductions in aboveground tree biomass from higher temperatures are roughly offset by increases in aboveground tree biomass from reductions in N and S deposition. However, under the higher climate change scenario (RCP 8.5) the decreases from climate change overwhelm increases from reductions in N and S deposition. These broad trends underlie wide variation among species. We found averaged across temperature scenarios the relative abundance of 60 species were projected to decrease more than 5% and 20 species were projected to increase more than 5%; and reductions of N and S deposition led to a decrease for 13 species and an increase for 40 species. This suggests large shifts in the composition of US forests in the future. Negative climate effects were mostly from elevated temperature and were not offset by scenarios with wetter conditions. We found that by 2100 an estimated 1 billion trees under the RCP 4.5 scenario and 20 billion trees under the RCP 8.5 scenario may be pushed outside the temperature record upon which these relationships were derived. These results may not fully capture future changes in forest composition as several other factors were not included. Overall efforts to reduce atmospheric deposition of N and S will likely be insufficient to overcome climate change impacts on forest demography across much of the United States unless we adhere to the low climate change scenario.

Decadal increase in groundwater inorganic carbon concentrations across Sweden

Groundwater is one of the largest continental carbon reservoirs and tightly linked to globally important carbon fluxes such as uptake on land, degassing from inland waters and delivery to oceans. Despite emerging evidence that these fluxes are sensitive to environmental changes, long-term carbon dynamics in groundwater remain widely unknown. Here I show that dissolved inorganic carbon and carbon dioxide concentrations in groundwater, calculated from environmental monitoring data (e.g. alkalinity, pH), have increased on average by 28% and 49%, respectively, across Sweden during 1980–2020. I attribute the observed changes mainly to a partial recovery from atmospheric sulfate deposition and associated shifts in weathering pathways, but also to enhanced soil respiration. The results highlight previously neglected long-term and large-scale dynamics in groundwater carbon cycling. These dynamics should be included in carbon cycle models for accurate evaluations and predictions of the effects of environmental changes on landscape and global carbon stocks and fluxes.

Ohio grain crop response to sulfur fertilization

AbstractContinuous declines in atmospheric sulfur (S) deposition along with increased S removal rates with crop harvest has the potential to lead to S deficiency in Ohio field crops. As a result, S fertilization has become more common over the past decade. However, the extent of S deficiency is unknown, as inherent soil properties and management practices influence S availability and uptake. We conducted 96 replicated trials, from 2013 to 2021 to (1) examine the response of corn (Zea mays L.), soybean [Glycine max (L.) Merr], and wheat (Triticum aestivum L.) to S application on a wide range of Ohio soils and differing management practices and (2) determine the ability of Mehlich‐3 extractable S in soil, leaf S, and grain S concentrations to predict grain yield response to S fertilizer. Our results showed limited grain yield increases to S fertilization with an overall response rate of 7.3% (4 of 50 corn trials, 3 of 34 soybean trials, and 0 of 12 wheat trials). Sulfur fertilization increased leaf and grain S concentrations by 19.4% and 12% in corn, by 22.2% and 7.7% in soybean, and by 41.7% and 0% in wheat, respectively. These increases in leaf or grain S concentrations were not directly related to yield responses. Diagnostic tools of Mehlich‐3 soil S, leaf S, and grain S concentrations failed to predict yield response to S. We conclude that S deficiency is not widespread in Ohio soils and that optimizing grain crop production does not currently require S fertilization.

Atmospheric wet deposition in urban and suburban sites across the United States

Compared to rural areas, there is a much poorer understanding of trends in wet atmospheric deposition across urban and suburban areas of the U.S. and how they compare to rural sites over time. The goal of this study was to investigate long-term trends in atmospheric wet deposition of nitrogen (ammonium and nitrate; NH4+ and NO3−), sulfate (SO42−), cations, and chloride (Cl−) for urban and suburban sites in the U.S. using data from the National Atmospheric Deposition Program (NADP) and to determine how long-term deposition trends relate to urbanization. For urban and suburban sites, we found that from the late 1970s to 2020, atmospheric deposition of NO3−, dissolved inorganic N (DIN), SO42−, hydrogen (H+), and magnesium (Mg2+) decreased over time, while deposition of NH4+ and potassium (K+) significantly increased over this period. When sites were categorized based on population density, we found no significant differences in rates of wet deposition between urban and background rural values, but the difference between urban and background rural values increased significantly over time for NO3− and DIN. When sites were categorized based on impervious surface area (ISA), we found that rates of NH4+, DIN, SO42, and calcium (Ca2+) deposition were significantly higher in urban sites (that had greater than 25% ISA) compared to background rural values. There were statistically significant positive relationships between population density and deposition of Mg2+, K+, sodium (Na+), and Cl− and significant positive relationships between % ISA and deposition of NO3− and Mg2+. Together, the results of this study demonstrate the urban enhancement of many forms of atmospheric deposition and the need for increased long-term monitoring of atmospheric deposition in cities and suburban sites throughout the U.S., especially in the western U.S.

Ecological Risks from Atmospheric Deposition of Nitrogen and Sulphur in Jack Pine forests of Northwestern Canada

Chronic elevated nitrogen (N) deposition can have adverse effects on terrestrial ecosystems. For large areas of northern Canada distant from emissions sources, long-range atmospheric transport of N may impact plant species diversity, even at low deposition levels. The objective of this study was to establish plant species community thresholds for N deposition under multiple environmental gradients using gradient forest analysis. Plant species abundance data for 297 Jack pine (Pinus banksiana Lamb.)-dominant forest plots across Alberta and Saskatchewan, Canada, were evaluated against 43 bioclimatic and deposition variables. Bioclimatic variables were overwhelmingly the most important drivers of community thresholds. Nonetheless, dry N oxide (DNO) and dry N dioxide deposition inferred a total deposited N (TDN) community threshold of 1.4–2.1 kg N ha−1 yr−1. This range was predominantly associated with changes in several lichen species, including Cladina mitis, Vulpicida pinastri, Evernia mesomorpha and Lecanora circumborealis, some of which are known bioindicators of N deposition. A secondary DNO threshold appeared to be driving changes in several vascular species and was equivalent to 2.45–3.15 kg N ha−1 yr−1 on the TDN gradient. These results suggest that in low deposition ‘background’ regions a biodiversity-based empirical critical load of 1.4–3.15 kg N ha−1 yr−1 will protect lichen communities and other N-sensitive species in Jack pine forests across Northwestern Canada. Nitrogen deposition above the critical load may lead to adverse effects on plant species biodiversity within these forests.

Sulfur fertiliser use in the Midwestern US increases as atmospheric sulfur deposition declines with improved air quality

Sulfur, as an essential nutrient for plant growth, has increasingly been used in fertiliser applications for many crops. This increase is coincident with declines in atmospheric sulfur deposition in response to air quality improvements in the United States and Europe. Here, we evaluate trends in sulfur fertiliser sales by mass, as a proxy for fertiliser applications, and estimate total atmospheric sulfur deposition across the Midwestern United States. Crop acreage, yield and sulfur fertiliser application substantially increased between 1985 and 2015, coincident with declines in atmospheric sulfur deposition. The increase in sulfur fertiliser has outpaced the relative rate of change in other major nutrient fertilisers including nitrogen, phosphorus and potassium, by approximately 7-fold prior to 2009, and 29-fold after 2009. We suggest that there is a critical need to develop sulfur management tools that optimize fertiliser applications to maintain crop yields while minimizing the consequences of excess sulfur in the environment.

Protection of forest ecosystems in the eastern United States from elevated atmospheric deposition of sulfur and nitrogen: A comparison of steady-state and dynamic model results

Critical loads (CLs) and target loads (TLs) of atmospheric deposition of sulfur (S) and nitrogen (N) specify the thresholds of air pollution above which damage to ecosystems is expected to occur and are used to inform environmental regulation and natural resource management. Model estimates of CL and TL can vary for a given location, and these differences can be important for characterization of ecosystem effects from elevated S and N deposition. Moreover, TLs are used to evaluate associated timeframes of ecosystem recovery. We compared published CLs and TLs based on soil acidity criteria derived from steady-state versus dynamic models for terrestrial ecosystems. We examined the magnitude of differences in the CL/TL results from the two types of models for the same regions in the Eastern U.S. Results showed that CLs/TLs from dynamic models (or from steady state modeling using soil base cation weathering estimates from dynamic models) generally produce a broader range of values of acid-sensitivity, including lower CLs/TLs, as compared with a steady-state approach. Applications of dynamic biogeochemical models capable of developing CLs/TLs are relatively data intensive and typically limited to locations where measured soil and soil solution (or nearby stream water) chemistry are available for model parameterization, calibration, and testing. We recommend that CLs/TLs derived from dynamic models be used, where data permit, as they are likely more accurate and allow for evaluation of time-dependent phenomena and period needed for recovery. However, CLs derived from steady-state models remain a useful tool for understanding broad spatial patterns in soil acid-sensitivity throughout the U.S. Future work should focus on the development of more reliable model input parameters, particularly soil base cation weathering, and the extent to which CLs and TLs at a given location may vary and be altered with anticipated future climate change. In addition, dynamic models could be further developed to estimate CLs/TLs for nutrient N.

Long-Term Experimental Manipulation of Atmospheric Sulfate Deposition to a Peatland: Response of Methylmercury and Related Solute Export in Streamwater.

Changes in sulfate (SO42-) deposition have been linked to changes in mercury (Hg) methylation in peatlands and water quality in freshwater catchments. There is little empirical evidence, however, of how quickly methyl-Hg (MeHg, a bioaccumulative neurotoxin) export from catchments might change with declining SO42- deposition. Here, we present responses in total Hg (THg), MeHg, total organic carbon, pH, and SO42- export from a peatland-dominated catchment as a function of changing SO42- deposition in a long-term (1998-2011), whole-ecosystem, control-impact experiment. Annual SO42- deposition to half of a 2-ha peatland was experimentally increased 6-fold over natural levels and then returned to ambient levels in two phases. Sulfate additions led to a 5-fold increase in monthly flow-weighted MeHg concentrations and yields relative to a reference catchment. Once SO42- additions ceased, MeHg concentrations in the outflow streamwater returned to pre-SO42- addition levels within 2 years. The decline in streamwater MeHg was proportional to the change in the peatland area no longer receiving experimental SO42- inputs. Importantly, net demethylation and increased sorption to peat hastened the return of MeHg to baseline levels beyond purely hydrological flushing. Overall, we present clear empirical evidence of rapid and proportionate declines in MeHg export from a peatland-dominated catchment when SO42- deposition declines.

Fifty years of reduction in sulphur deposition drives recovery in soil pH and plant communities

Abstract Sulphur deposition through rainfall has led to species loss and ecosystem degradation globally, and across Europe huge reductions in sulphur emissions since the 1970s were expected to promote the recovery of acidified ecosystems. However, the rate and ecological impact of recovery from acidification in terrestrial ecosystems is still unclear as is the influence of management and climate, as to date there has been no long‐term spatially extensive evaluation of these changes. Here, we present data from thousands of sites across Great Britain (pH range 3.3–8.7) surveyed repeatedly from 1978–2019 and assess change in soil pH and plant acidity preference (Ellenberg R) in response to atmospheric deposition of sulphur and nitrogen. We analyse change in grasslands managed for pasture, referred to as high‐intensity habitats, and compare to seminatural habitats comprising rough grassland, broadleaved woodland, bog and heathland, referred to as low‐intensity habitats. Soil pH increased from 1978 to 2007 but then decreased between 2007 and 2019, resulting in a net increase of ~0.2 pH units in low‐intensity habitats but no change in high‐intensity habitats. The community average Ellenberg R increased in seminatural habitats by ~0.2 units but remained stable in intensive grasslands. In seminatural habitats, but not intensive grasslands, these changes in plant community composition were associated with the soil pH changes which were in turn linked to decreasing sulphur deposition and differences in rainfall. Nitrogen deposition, which was relatively stable over the survey period, showed no additional effect upon soil acidity once sulphur deposition was accounted for. Synthesis: Our results provide conclusive evidence that reductions in acid emissions are stimulating the gradual recovery of chronically acidified terrestrial ecosystems at a whole‐country scale, while also suggesting this recovery is being compromised by changing climate and land management.

Long-term declines in atmospheric nitrogen and sulfur deposition reduce critical loads exceedances at multiple Canadian rural sites, 2000–2018

Abstract. Daily air concentrations of inorganic nitrogen (N) species, including gaseous HNO3 and particulate-bound (p)NH4+ and pNO3-, and sulfur (S) species, including SO2 and pSO42-, and precipitation concentrations of NO3-, NH4+, and SO42-, have been routinely monitored by the Canadian Air and Precipitation Monitoring Network (CAPMoN) since 1983. Data at 15 rural sites from 2000–2018 were used to estimate dry and wet N and S deposition fluxes, which were then used to explore their spatiotemporal trends and assess ecosystem damage through a retrospective analysis of critical loads (CLs) exceedances. Total (dry + wet) N deposition ranged from 1.7–9.5 kgNha-1yr-1 among the 15 sites, though dry deposition of NH3 and some oxidized N species were not included due to lack of monitoring data. Based on additional N measurements in 2010 at one of the sites, annual total N deposition may be underestimated by up to 32 %. Total N deposition was dominated by wet NO3- and wet NH4+ deposition, which together comprised 71 %–95 %. Contributions to dry N deposition were 40 %–74 % by HNO3, 11 %–40 % by pNH4+, and 5 %–25 % by pNO3-. Total S deposition ranged from 1.3–8.5 kgSha-1yr-1 and was dominated by wet deposition of SO42- and dry deposition of SO2. Relative percentages of wet and dry S deposition were 45 %–89 % and 11 %–55 %, respectively. Acidic ion fluxes were greatest in southeastern Canada and were comparable among the west coast, prairie, remote, and eastern Canadian sites. Oxidized N (dry HNO3, dry pNO3-, wet NO3-) deposition was greater than that of reduced N (dry pNH4+, wet NH4+) in the early 2000s. In 2014–2018, reduced N deposition surpassed that of oxidized N in southeastern Canada. Total N and S deposition decreased significantly at a rate of −0.03 to −0.25 kgNha-1yr-1 (−1.1 % yr−1 to −3.3 % yr−1) and −0.08 to −0.66 kgSha-1yr-1 (−3.5 % yr−1 to −6.6 % yr−1), respectively, among the sites. The weak declining trend in total N deposition at the west coast site was consistent with the slower decline in NOx emissions in western Canada. Reductions in total N deposition were driven by its oxidized form as trends in reduced N were non-significant. As a result, reduced N contributions to total N deposition increased on average from 42 % in 2000–2004 to 53 % in 2014–2018. Anthropogenic NOx and SO2 emissions reductions in both eastern Canada and eastern US were highly effective in reducing total oxidized N and total S deposition, respectively, in eastern Canada. Acidic deposition exceeded terrestrial CL at 5 of the 14 sites and aquatic CL at 2 of the 5 sites in the early 2000s. However, exceedances have been trending downwards and acidic deposition fluxes were mostly near or below CL after 2012 for the subset of sites assessed, which support recovery from historical acidification. Further assessments of CL exceedances are required in other Canadian regions susceptible to acidification and affected by elevated or increasing N and S emissions.

Deforestation alters dissolved organic carbon and sulfate dynamics in a mountainous headwater catchment—A wavelet analysis

Deforestation has a wide range of effects on hydrological and geochemical processes. Dissolved organic carbon (DOC) dynamics, a sensitive environmental change indicator, is expected to be affected by deforestation, with changes in atmospheric sulfur (S) deposition compounding this. However, how precisely anthropogenic disturbance (deforestation) under a declining atmospheric S input scenario affects the underlying spatiotemporal dynamics and relationships of river DOC and sulfate with hydro-climatological variables e.g., stream water temperature, runoff, pH, total dissolved iron (Fetot), and calcium (Ca2+) remains unclear. We, therefore, examined this issue within the TERENO Wüstebach catchment (Eifel, Germany), where partial deforestation had taken place in 2013. Wavelet transform coherence (WTC) analysis was applied based on a 10-year time series (2010–2020) from three sampling stations, whose (sub) catchment areas have different proportions of deforested area (W10: 31%, W14: 25%, W17: 3%). We found that water temperature and DOC, sulfate, and Fetot concentrations showed distinct seasonal patterns, with DOC averaging concentrations ranging from 2.23 (W17) to 4.56 (W10) mg L–1 and sulfate concentration ranging from 8.04 (W10) to 10.58 (W17) mg L–1. After clear-cut, DOC significantly increased by 59, 58% in the mainstream (W10, W14), but only 26% in the reference stream. WTC results indicated that DOC was negatively correlated with runoff and sulfate, but positively correlated with temperature, Ca2+, and Fetot. The negative correlation between DOC with runoff and sulfate was apparent over the whole examined 10-year period in W17 but did end in W10 and W14 after the deforestation. Sulfate (SO4) was highly correlated with stream water temperature, runoff, and Fetot in W10 and W14 and with a longer lag time than W17. Additionally, pH was stronger correlated (higher R2) with sulfate and DOC in W17 than in W10 and W14. In conclusion, WTC analysis indicates that within this low mountainous forest catchment deforestation levels over 25% (W10 and W14) affected the coupling of S and C cycling substantially more strongly than “natural” environmental changes as observed in W17.