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Background: Fine particulate matter (PM2.5) has been widely associated with airway inflammation represented by increased fractional concentration of exhaled nitric oxide (FeNO). However, it remains unclear whether various PM2.5 constituents have different impacts on FeNO and its production process from the arginase (ARG)–nitric oxide synthase (NOS) pathway. Objectives: To investigate the acute effects of PM2.5 constituents on FeNO and DNA methylation of genes involved. Methods: We conducted a longitudinal panel study among 43 young adults in Shanghai, China from May to October in 2016. We monitored the concentrations of 25 constituents of PM2.5. We applied the linear mixed-effect model to evaluate the associations of PM2.5 constituents with FeNO and DNA methylation of the ARG2 and NOS2A genes. Results: Following PM2.5 exposure, NOS2A methylation decreased and ARG2 methylation increased only on the concurrent day, whereas FeNO increased most prominently on the second day. Nine constituents (OC, EC, K, Fe, Zn, Ba, Cr, Se, and Pb) showed consistent associations with elevated FeNO and decreased NOS2A methylation or increased ARG2 methylation in single-constituent models and models adjusting for PM2.5 total mass and collinearity. An interquartile range increase of these constituents was associated with respective decrements of 0.27–1.20 in NOS2A methylation (%5mC); increments of 0.48–1.56 in ARG2 methylation (%5mC); and increments of 7.12%–17.54% in FeNO. Conclusions: Our results suggested that OC, EC, and some metallic elements may be mainly responsible for the development and epigenetic regulation of airway inflammatory response induced by short-term PM2.5 exposure. Keywords: Fine particulate matter, Chemical constituents, Airway inflammation, Exhaled nitric oxide, DNA methylation, Panel study

Nitrate aerosol plays an increasingly important role in wintertime haze pollution in China. Despite intensive research on the wintertime nitrate chemistry in recent years, quantitative constraints on the formation mechanisms of nitrate aerosol in the Yangtze River Delta (YRD), one of the most developed and densely populated regions in eastern China, remain inadequate. In this study, we identify the major nitrate formation pathways and their key controlling factors during the winter haze pollution period in the eastern YRD using two-year (2018-2019) field observations and detailed observation-constrained model simulations. We find that the high atmospheric oxidation capacity, coupled with high aerosol liquid water content (ALWC), made both the heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) and the gas-phase OH oxidation of nitrogen dioxide (NO2) important pathways for wintertime nitrate formation in this region, with contribution percentages of 69% and 29% in urban areas and 63% and 35% in suburban areas, respectively. We further find that the gas-to-particle partitioning of nitric acid (HNO3) was very efficient so that the rate-determining step in the overall formation process of nitrate aerosol was the oxidation of NOx to HNO3 through both heterogeneous and gas-phase processes. The atmospheric oxidation capacity (i.e., the availability of O3 and OH radicals) was the key factor controlling the production rate of HNO3 from both processes. During the COVID-19 lockdown (January-February 2020), the enhanced atmospheric oxidation capacity greatly promoted the oxidation of NOx to nitrate and hence weakened the response of nitrate aerosol to the emission reductions in urban areas. Our study sheds light on the detailed formation mechanisms of wintertime nitrate aerosol in the eastern YRD and highlights the demand for the synergetic regulation of atmospheric oxidation capacity and NOx emissions to mitigate wintertime nitrate and haze pollution in eastern China. [ABSTRACT FROM AUTHOR]

Mercury (Hg) is a global toxic pollutant that can be released into the atmosphere through anthropogenic and natural sources. The uncertainties in the estimated emission amounts are much larger from natural than anthropogenic sources. A method was developed in the present study to quantify the contributions of natural surface mercury emissions to ambient gaseous elemental mercury (GEM) concentrations through application of positive matrix factorization (PMF) analysis with temperature, O[sub 3], and NH3 as indicators of GEM emissions from natural surfaces. GEM concentrations were continuously monitored at a 2-hourly resolution at a regional background site in the Yangtze River Delta in Eastern China during 2015-2018. Annual average GEM concentrations were in the range of 2.03-3.01 ng/m³, with a strong decreasing trend at a rate of-0.32 ± 0.07 ng m[sup -3] yr-1 from 2015 to 2018, which was mostly caused by reduced anthropogenic emissions since 2013. The estimated contributions from natural surface emissions of mercury to the ambient GEM concentrations were in the range of 0.90-1.01 ng/m³ on annual average with insignificant interannual changes, but the relative contribution increased significantly from 36% in 2015 to 53% in 2018, gradually surpassing those from anthropogenic sources. [ABSTRACT FROM AUTHOR]