Spatial distribution and seasonal variations of atmospheric sulfur deposition over Northern China

Abstract. The increasing anthropogenic emissions of acidic compounds have induced acid deposition accompanied by acidification in the aquatic and terrestrial ecosystems worldwide. However, comprehensive assessment of spatial patterns and long-term trends of acid deposition in China remains a challenge due to a paucity of field-based measurement data, in particular for dry deposition. Here we quantify the sulfur (S) deposition on a regional scale via precipitation, particles and gases during a 3-yr observation campaign at ten selected sites in Northern China. Results show that the total S deposition flux in the target area ranged from 35.0 to 100.7 kg S ha−1 yr−1, categorized as high levels compared to those documented in Europe, North America, and East Asia. The ten-site, 3-yr average total S deposition was 64.8 kg S ha−1 yr−1, with 32% attributed to wet deposition, and the rest attributed to dry deposition. Compared with particulate sulfate, gaseous SO2 was the major contributor of dry-deposited S, contributing approximately 49% to the total flux. Wet deposition of sulfate showed pronounced seasonal variations with maximum in summer and minimum in winter, corresponding to precipitation patterns in Northern China. However, the spatial and inter-annual differences in the wet deposition were not significant, which were influenced by the precipitation amount, scavenging ratio and the concentrations of atmospheric S compounds. In contrast, the relatively large dry deposition of SO2 and sulfate during cold season, especially at industrial areas, was reasonably related to the local emissions from home heating. Although seasonal fluctuations were constant, clear spatial differences were observed in the total S deposition flux and higher values were also found in industrial areas with huge emissions of SO2. These findings indicate that human activity has dramatically altered the atmospheric S deposition and thus regional S cycles. To systematically illustrate the potential effects of acidifying deposition on the receiving environment, we calculated the deposition of "potential acidity" that takes into account the microbial transformation of ammonium to nitrate in the ecosystems, resulting in the release of hydrogen ions. The estimated total "acid equivalents" deposition of S and nitrogen (N) fell within the range of 4.2–11.6 keq ha−1 yr−1, with a ten-site, 3-yr mean of 8.4 keq ha−1 yr−1. This value is significantly higher than that of other regions in the world and exceeds the critical loads for natural ecosystems in Northern China, thus prompting concerns regarding ecological impacts. The contribution of S to total acid deposition was comparable to that of N at most of sites; however, the importance of S on acidification risks was more pronounced in the industrial sites, highlighting that further SO2 abatement from industrial emissions is still needed. Taking these findings and our previous studies together, a multi-pollutant perspective and joint mitigate strategies to abate SO2 and NH3 simultaneously in the target areas are recommended to protect the natural ecosystems from excess acid deposition caused by anthropogenic emissions.