This study incorporated stable isotope analyses with chemical analyses to determine the origin and migration of sulfur sources in East Asia, and these findings were compared with our decadal research from 2000 to 2001 and 2002 to 2003. The multiple sulfur isotope composition (32S, 33S and 34S) of the dissolved sulfate in precipitation was first measured from 2011 to 2013 in Seoul, South Korea. The δ34Snss values were −1.1‰ to 7.9‰ (avg. 3.6‰), strongly suggesting that sulfur derived from the combustion of Chinese coal is the predominant source of sulfate in the Seoul region. Low NO3/SO42− ratios in the precipitation samples indicated an insignificant effect of sulfur from vehicle exhaust. The seasonal variation of δ34Snss values appears to be caused by increasing biogenic sulfur activity during the spring and summer seasons. The some Δ33S values (0.13‰–0.16‰) measured in the three samples were sufficiently small; thus, whether these values can be attributed to mass-independent fractionation remains unclear. Measuring the Δ33S anomalies in dissolved sulfate provides valuable insights for identifying the sources of sulfur transferred from the stratosphere to the troposphere and upper troposphere.

In this study, ozonesonde data were used to evaluate the impact of different boundary conditions on the vertical distribution of ozone over urban Beijing. The comparison shows that the clean and static boundary conditions, referred to as PROFILE, apparently underestimate the ozone concentration over the upper troposphere and stratosphere, whereas the global chemical transport model (CTM) provides much more reasonable performance. Further investigation reveals that the boundary conditions exert larger impacts over areas with high altitudes and close distances to boundaries, such as the Tibetan Plateau, while they yield weak impacts on regions relatively far from the boundary, such as the North China Plain (NCP). Process analysis was conducted to investigate the modulation of physical and chemical processes on ozone formation in June 2017, illustrating that during the daytime of the high-O₃ period, the photochemical reactions within the planetary boundary layer (PBL) almost become the only source favorable to ozone accumulation. Motivated by this phenomenon, we constructed a linear regression and found that the maximum daily 8-hr ozone (MDA8) ozone concentration was highly correlated with the surface ozone change rate and chemical reactions in the PBL during the pollution period, with MDA8 ozone exceeding 70 ppbv over NCP. Based on this relationship as well as the design of numerical experiments, we propose a strategy of dynamic emission control. Firstly, the emission reduction during the peak ozone formation period may weaken the fast chemical reactions in the PBL and subsequent surface ozone concentration. Secondly, emission reduction one or two days prior to an episode might achieve larger ozone reduction through the accumulation effect. Lastly, emission control outside of the NCP may surpass the local impact under favorable meteorological conditions. Therefore, the efficacy of dynamic emission control was striking when both the accumulation and transport effect were taken into consideration.

The specific activities of natural (²¹⁰Pb, ²²⁶Ra, and ²³²Th) and artificial (¹³⁷Cs, ²³⁹,²⁴⁰Pu, and ²⁴¹Am) radionuclides in the sediments of two North Caucasus lakes were determined. The two lakes, Lake Khuko and Lake Donguz-Orun, differ in their sedimentation conditions. Based on the use of unsupported ²¹⁰Pbₑₓ and both Chernobyl-derived and bomb-derived ¹³⁷Cs as chronological markers, it was established that the sedimentation rates in Lake Khuko over the past 55–60 y did not exceed 0.017 cm y⁻¹. Sedimentation rates in Lake Donguz-Orun were found to be more than an order of magnitude higher. In the latter case, the sedimentation rates for the period from 1986 to the present were over 1.5 times higher than they were for the period 1963–1986. The differences in sedimentation rates were due to differences in the rates of denudation of their respective catchment areas. The specific activities of artificial radionuclides (¹³⁷Cs, 2600 Bq kg⁻¹; ²³⁹,²⁴⁰Pu, 162 Bq kg⁻¹; and ²⁴¹Am, 36 Bq kg⁻¹) and their ratios in the sediments of Lake Khuko show that their deposition was mainly due to global stratospheric fallout of technogenic radionuclides associated with nuclear bomb testing during 1954–1963—rather than fallout from the Chernobyl accident. Several factors, including the mode of precipitation, features of the surface runoff, and location of Lake Khuko, were responsible for the accumulation of artificial radionuclides.

Agriculture is one of major emission sources of nitrous oxide (N₂O), an important greenhouse gas dominating stratospheric ozone destruction. However, indirect N₂O emissions from agriculture watershed water surfaces are poorly understood. Here, surface-dissolved N₂O concentration in water bodies of the agricultural watershed in Eastern China, one of the most intensive agricultural regions, was measured over a two-year period. Results showed that the dissolved N₂O concentrations varied in samples taken from different water types, and the annual mean N₂O concentrations for rivers, ponds, reservoir, and ditches were 30 ± 18, 19 ± 7, 16 ± 5 and 58 ± 69 nmol L⁻¹, respectively. The N₂O concentrations can be best predicted by the NO3−-N concentrations in rivers and by the NH4+-N concentrations in ponds. Heavy precipitation induced hot moments of riverine N₂O emissions were observed during farming season. Upstream waters are hot spots, in which the N₂O production rates were two times greater than in non-hotspot locations. The modeled watershed indirect N₂O emission rates were comparable to direct emission from fertilized soil. A rough estimate suggests that indirect N₂O emissions yield approximately 4% of the total N₂O emissions yield from N-fertilizer at the watershed scale. Separate emission factors (EF) established for rivers, ponds, and reservoir were 0.0013, 0.0020, and 0.0012, respectively, indicating that the IPCC (Inter-governmental Panel on Climate Change) default value of 0.0025 may overestimate the indirect N₂O emission from surface water in eastern China. EF was inversely correlated with N loading, highlighting the potential constraints in the IPCC methodology for water with a high anthropogenic N input.

The consequence of the lockdowns implemented to address the COVID-19 pandemic on human health damage due to air pollution and other environmental issues must be better understood. This paper analyses the effect of reducing energy demand on the evolution of environmental impacts during the occurrence of 2020-lockdown periods in Italy, with a specific focus on life expectancy. An energy metabolism analysis is conducted based on the life cycle assessment (LCA) of all monthly energy consumptions, by sector, category and province area in Italy between January 2015 to December 2020. Results show a general decrease (by ∼5% on average) of the LCA midpoint impact categories (global warming, stratospheric ozone depletion, fine particulate matter formation, etc.) over the entire year 2020 when compared to past years. These avoided impacts, mainly due to reductions in fossil energy consumptions, are meaningful during the first lockdown phase between March and May 2020 (by ∼21% on average). Regarding the LCA endpoint damage on human health, ∼66 Disability Adjusted Life Years (DALYs) per 100,000 inhabitants are estimated to be saved. The analysis shows that the magnitude of the officially recorded casualties is substantially larger than the estimated gains in human lives due to the environmental impact reductions. Future research could therefore investigate the complex cause-effect relationships between the deaths occurred in 2020 imputed to COVID-19 disease and co-factors other than the SARS-CoV-2 virus.

Microbial denitrification is a main source of nitrous oxide (N₂O) emissions which have strong greenhouse effect and destroy stratospheric ozone. Though the importance of sulfide driven chemoautotrophic denitrification has been recognized, its contribution to N₂O emissions in nature remains elusive. We built up long-term sulfide-added microcosms with sediments from two freshwater lakes. Chemistry analysis confirmed sulfide could drive nitrate respiration in long term. N₂O accumulated to over 1.5% of nitrate load in both microcosms after long-term sulfide addition, which was up to 12.9 times higher than N₂O accumulation without sulfide addition. Metagenomes were extracted and sequenced during microcosm incubations. 16 S rRNA genes of Thiobacillus and Defluviimonas were gradually enriched. The nitric oxide reductase with c-type cytochromes as electron donors (cNorB) increased in abundance, while the nitric oxide reductase receiving electrons from quinols (qNorB) decreased in abundance. cnorB genes similar to Thiobacillus were enriched in both microcosms. In parallel, enrichment was observed for enzymes involved in sulfur oxidation, which supplied electrons to nitrate respiration, and enzymes involved in Calvin Cycle, which sustained autotrophic cell growth, implying the coupling relationship between carbon, nitrogen and sulfur cycling processes. Our results suggested sulfur pollution considerably increased N₂O emissions in natural environments.

Volatile brominated compounds are important trace gases for stratospheric ozone chemistry. In this study, the spatial variations of dibromomethane (CH₂Br₂), bromodichloromethane (CHBrCl₂), dibromochloromethane (CHBr₂Cl) and bromoform (CHBr₃) in the seawater and overlying atmosphere were measured in the Yellow Sea (YS) and the East China Sea (ECS) in winter. The air-sea fluxes of CH₂Br₂, CHBrCl₂, CHBr₂Cl and CHBr₃ ranged from −11.46 to 25.33, −4.68 to 7.91, −8.60 to 4.08 and −88.57 to 8.84 nmol m⁻²·d⁻¹, respectively. In order to understand the mechanism of halocarbons production, we measured bromoperoxidase (BrPO) activity (39.18–186.74 μU·L⁻¹) in the YS and ECS for the first time using an aminophenyl fluorescein (APF) method and performed in-situ incubation experiments in BrPO-treated seawater. The production rates of CH₂Br₂, CHBrCl₂, CHBr₂Cl and CHBr₃ ranged from 14.21 to 94.74, 0.00 to 19.74, 0.00 to 30.62 and 6.18–72.75 pmol L⁻¹·h⁻¹, respectively, in BrPO-treated seawater. There were significantly higher production rates in coastal waters compared with the open sea (P = 0.016) because of higher DOC levels near the coast. Moreover, the production rates of halocarbons increased with BrPO activity and H₂O₂ concentration. The results showed that enzyme-mediated reaction was an important source for the production of halocarbons in seawater. The present research is of great significance for understanding the production mechanisms of halocarbons in seawater and global oceanic halocarbons emissions.

Inorganic particulate nitrate (p-NO3−), gaseous nitric acid (HNO₃₍g₎) and nitrogen oxides (NOₓ = NO + NO₂), as main atmospheric pollutants, have detrimental effects on human health and aquatic/terrestrial ecosystems. Referred to as the ‘Third Pole’ and the ‘Water Tower of Asia’, the Tibetan Plateau (TP) has attracted wide attention on its environmental changes. Here, we evaluated the oxidation processes of atmospheric nitrate as well as traced its potential sources by analyzing the isotopic compositions of nitrate (δ¹⁵N, δ¹⁸O, and Δ¹⁷O) in the aerosols collected from the Mt. Everest region during April to September 2018. Over the entire sampling campaigns, the average of δ¹⁵N(NO3−), δ¹⁸O(NO3−), and Δ¹⁷O(NO3−) was −5.1 ± 2.3‰, 66.7 ± 10.2‰, and 24.1 ± 3.9‰, respectively. The seasonal variation in Δ¹⁷O(NO3−) indicates the relative importance of O₃ and HO₂/RO₂/OH in NOₓ oxidation processes among different seasons. A significant correlation between NO3− and Ca²⁺ and frequent dust storms in the Mt. Everest region indicate that initially, the atmospheric nitrate in this region might have undergone a process of settling; subsequently, it got re-suspended in the dust. Compared with the Δ¹⁷O(NO3−) values in the northern TP, our observed significantly higher values suggest that spatial variations in atmospheric Δ¹⁷O(NO3−) exist within the TP, and this might result from the spatial variations of the atmospheric O₃ levels, especially the stratospheric O₃, over the TP. The observed δ¹⁵N(NO3−) values predicted remarkably low δ¹⁵N values in the NOₓ of the sources and the N isotopic fractionation plays a crucial role in the seasonal changes of δ¹⁵N(NO3−). Combined with the results from the backward trajectory analysis of air mass, we suggest that the vehicle exhausts and agricultural activities in South Asia play a dominant role in determining the nitrate levels in the Mt. Everest region.

Nitrous oxide (N2O) is a potent greenhouse gas that contributes to climate change and stratospheric ozone destruction. Nitrogen-enriched rivers are significant sources of atmospheric N2O. This study conducted a one-year field campaign in seven N-enriched rivers draining urban, rural, and agricultural land to determine the link between the production, concentrations, and emissions of N2O and land use. Estimated N2O fluxes varied between 1.30 and 1164.38 μg N2O-N m−2 h−1 with a mean value of 154.90 μg N2O-N m−2 h−1, indicating that rivers were the net sources of atmospheric N2O. Concentrations of N2O ranged between 0.23 and 29.21 μg N2O-N L−1 with an overall mean value of 3.81 μg N2O-N L−1. Concentrations of ammonium and nitrate in urban and rural rivers were high in the cold season. The concentrations were also high in agricultural rivers in the wet season. N2O concentrations and emissions in rural and urban rivers followed a similar pattern to ammonium and a similar pattern to nitrate in agricultural rivers. A strong link between the concentrations and emissions of N2O and land use was observed. N2O concentrations in and emissions from the rivers draining the urban and rural areas were significantly higher than the rivers draining the agricultural areas (P < 0.01). Stepwise regression analysis indicated that dissolved N2O were primarily influenced by NH4+ in agricultural rivers and by NO3− in rural rivers; while dissolved N2O in urban rivers was primarily predicted by temperature and reflected the integrated impact of sewage input and river hydrology. Nitrate-N and NO3--O isotope data and linear regression of N2O and river water variables strongly indicated that dissolved N2O was mainly derived from nitrification in agricultural rivers and denitrification in rural and urban rivers.

The oxidizing capacity of the atmosphere, defined as the global mean tropospheric abundance of the hydroxyl radical (OH·), strongly influences air pollution by controlling the lifetimes of gaseous pollutants and the production of particulate matter. Predicting future changes in OH· due to anthropogenic emissions and climate change is of interest to air quality managers, but it is difficult because of multiple competing effects. Models of atmospheric chemistry suggest that these competing effects buffer significant change in OH· in the past and in the near future. However, proxy-based observations for past changes in OH· and other oxidants over the preindustrial-industrial and glacial-interglacial time scales suggest much larger changes than models estimate. Model sensitivity studies show that variability in past and future OH· is highly sensitive to relative emissions of reactive nitrogen and carbon, water vapor, lightning, and stratospheric ozone, implying that one or more of these variables is highly sensitive to climate.