ABSTRACT
It is increasingly clear that increases in dissolved organic carbon in upland waters in recent decades have often been dominated by acid deposition, but reasons for substantial variation in rates of change remain unclear. This paper focuses on the extent to which spatial properties, such as variation in soil properties, atmospheric deposition and climate, affect the sensitivity of DOC concentrations in soil water. The purpose is to i) examine evidence for differences in site average concentrations and trends in soil water DOC between sites with contrasting ecosystem properties, i.e. vegetation cover and soil type, and ii) identify the wider combination of site characteristics that best explain variation in these DOC metrics between sites. We collated soil water and deposition chemistry, soil chemistry and meteorological data from 15 long-term UK monitoring sites (1992-2010) covering a range of soils, vegetation, climate and acid deposition levels. Mineral soils under forests showed the greatest range of long-term mean DOC concentrations and trends. Regression analysis indicated that acid and sea-salt deposition, and soil sensitivity to acidification were the factors most strongly associated with spatial variation in mean DOC concentrations. Spatial variation in DOC trends were best explained by Al saturation and water flux. Overall, the sensitivity of DOC release from soil to changes in pollutant deposition could be related to the type of vegetation cover and soils chemistry properties, such as Al saturation, divalent base cation content and hydrological regime. The identification of the ecosystem properties that appear most influential in modifying DOC production and responses to long-term drivers, helps elucidate potential mechanistic explanations for differences in DOC dynamics across seemingly similar ecosystems, and points to the importance of DOC mobility in regulating its dynamics.
ABSTRACT
There is emerging concern over the impact of extreme events such as heavy rainfall on the quality of water entering the drinking water supply from aboveground sources, as such events are expected to increase in magnitude and frequency in response to climate change. We compared the impact of rainfall events on streamwater quality in four contrasting upland (peatland and mineral soil) and lowland agricultural catchments used to supply drinking water in France (Brittany) and the United Kingdom (North Wales) by analyzing water samples collected before, during, and after specific events. At all four streams, heavy rainfall led to a considerable rise in organic matter concentration ranging from 48 to 158%. Dissolved organic carbon (DOC) quality, as determined using specific ultraviolet absorbance, changed consistently at all sites during rainfall events, with a greater proportion of aromatic and higher molecular weight compounds following the onset of rainfall. However, the change in DOC quality and quantity did not significantly alter the trihalomethane formation potential. We observed small increases in trihalomethane (THM) generation only at the Welsh peatland and agricultural sites and a small decrease at the Brittany agricultural site. The proportion of brominated THMs in chlorinated waters was positively correlated with bromide/DOC ratio in raw waters for all sites and hydrological conditions. These results provide a first indication of the potential implications for surface-based drinking water resources resulting from expected future increases in rainfall event intensity and extension of dry periods with climate changes.
ABSTRACT
Anthropogenically derived nitrogen (N) has a central role in global environmental changes, including climate change, biodiversity loss, air pollution, greenhouse gas emission, water pollution, as well as food production and human health. Current understanding of the biogeochemical processes that govern the N cycle in coupled human-ecological systems around the globe is drawn largely from the long-term ecological monitoring and experimental studies. Here, we review spatial and temporal patterns and trends in reactive N emissions, and the interactions between N and other important elements that dictate their delivery from terrestrial to aquatic ecosystems, and the impacts of N on biodiversity and human society. Integrated international and long-term collaborative studies covering research gaps will reduce uncertainties and promote further understanding of the nitrogen cycle in various ecosystems.
Subject(s)
Biodiversity , Ecosystem , Nitrogen Cycle , Climate ChangeABSTRACT
Research on the ecosystem impacts of acidifying pollutants, and measures to control them, has focused almost exclusively on sulfur (S) and nitrogen (N) compounds. Hydrochloric acid (HCl), although emitted by coal burning, has been overlooked as a driver of ecosystem change because most of it was considered to redeposit close to emission sources rather than in remote natural ecosystems. Despite receiving little regulatory attention, measures to reduce S emissions, and changes in energy supply, have led to a 95% reduction in United Kingdom HCl emissions within 20 years. Long-term precipitation, surface water, and soil solution data suggest that the near-disappearance of HCl from deposition could account for 30-40% of chemical recovery from acidification during this time, affecting both near-source and remote areas. Because HCl is highly mobile in reducing environments, it is a more potent acidifier of wetlands than S or N, and HCl may have been the major driver of past peatland acidification. Reduced HCl loadings could therefore have affected the peatland carbon cycle, contributing to increases in dissolved organic carbon leaching to surface waters. With many regions increasingly reliant on coal for power generation, HCl should be recognized as a potentially significant constituent of resulting emissions, with distinctive ecosystem impacts.
Subject(s)
Air Pollutants/chemistry , Hydrochloric Acid/chemistry , Air Pollutants/analysis , Air Pollutants/toxicity , Air Pollution/statistics & numerical data , Carbon Cycle/drug effects , Chlorine/analysis , Ecosystem , Environment , Environmental Monitoring , Fresh Water/chemistry , Hydrochloric Acid/analysis , Hydrochloric Acid/toxicity , Hydrogen-Ion Concentration , Soil/chemistryABSTRACT
In the United Kingdom, as in other regions of Europe and North America, recent decreases in surface water sulphate concentrations, due to reduced sulphur emissions, have coincided with marked increases in dissolved organic carbon (DOC) concentrations. Since many of the compounds comprising DOC are acidic, the resulting increases in organic acidity may have the potential to offset the benefits of a decrease in mineral (sulphate) acidity. To test this, we used a triprotic model of organic acid dissociation to estimate the proportional organic acid buffering of reduced mineral acidity as measured in the 22 lakes and streams monitored by the UK Acid Waters Monitoring Network. For an average non-marine sulphate decrease of 30 mueq l(-1) over 15 years from 1988-2003, we estimate that around 28% was counterbalanced by rising strong organic acids, 20% by rising alkalinity (partly attributable to an increase in weak organic acids), 11% by falling inorganic aluminium and 41% by falling non-marine base cations. The situation is complicated by a concurrent decrease in marine ion concentrations, and the impact this may have had on both DOC and acidity, but results clearly demonstrate that organic acid increases have substantially limited the amount of recovery from acidification (in terms of rising alkalinity and falling aluminium) that have resulted from reducing sulphur emissions. The consistency and magnitude of sulphate and organic acid changes are consistent with a causal link between the two, possibly due to the effects of changing acidity, ionic strength and aluminium concentrations on organic matter solubility. If this is the case, then organic acids can be considered effective but partial buffers to acidity change in organic soils, and this mechanism needs to be considered in assessing and modelling recovery from acidification, and in defining realistic reference conditions. However, large spatial variations in the relative magnitude of organic acid and sulphate changes, notably for low-deposition sites in northwestern areas where organic acid increases apparently exceed non-marine sulphate decreases, suggest that additional factors, such as changes in sea-salt deposition and climatic factors, may be required to explain the full magnitude of DOC increases in UK surface waters.