Spatial and temporal variation of inorganic ions in rainwater in Sichuan province from 2011 to 2016.

China continues to suffer from severe acid deposition, despite the government implying a series of policies to control air pollution. In this study, rainwater samples were collected from 2011 to 2016 in Sichuan province to measure the pH values and the concentrations of nine inorganic ions (SO42-, NO3-, NH4+, Cl-, Na+, Ca2+, K+, Mg2+, and F-), and then to investigate their spatiotemporal variations. Besides, the dominant sources for the acidic ions in the precipitation were also revealed by statistical model. The results showed that the rainwater continued to be highly acidic, and the Volume-Weighted Mean (VWM) pH value was calculated to be 5.18 during 2011 and 2016. NH4+, Ca2+, NO3-, and SO42- were the dominant water-soluble inorganic ions, accounting for 79.2% of the total ions on average. The remarkable decrease in NO3- and SO42- concentrations (from 75.9 to 54.3 μeq L-1 and from 285 to 145 μeq L-1, respectively) resulted in an increase in the pH value of rainwater from 5.24 in 2011 to 5.70 in 2016. The concentrations of SO42-, NO3-, F-, Na+, and K+ showed remarkably seasonal variation, with the highest value observed in winter, followed by spring and autumn, and the lowest value observed in summer. High VWM concentration of these ions in winter were mainly due to adverse meteorological conditions (e.g., rare rainfall, lower planetary boundary height, and stagnant air) and intensive anthropogenic emissions. SO42-, NO3-, and F- ions peaked in the southeastern Sichuan province, which is a typical industrial region. NH4+ concentrations decreased from 268 μeq L-1 in the east to 10.4 μeq L-1 in the western Sichuan province, which could be related to the development of agriculture in the eastern Sichuan province. Ca2+ peaked in southeastern Sichuan province due to intensive construction activities and severe stone desertification. On the basis of Positive Matrix Factorization (PMF) analysis, four sources of inorganic ions in rainwater were identified, including anthropogenic source, crust, biomass burning, and aging sea salt aerosol. Geographically Weighted Regression (GWR) was used to find the spatial correlations between the socio-economic factors and ions in the rainwater. At the regional scale, the influence of fertilizer consumption and Gross Agricultural Production (GAP) on NH4+ increased from east to west; moreover the influence of Gross Industrial Production (GIP) on SO42- and NO3- also increased.