This study reveals aerosol liquid water content (ALWC) in PM2.5 ranged from 2% up to 74%, and the associated secondary inorganic fraction rose from 24% to 55%, while ambient relative humidity (RH) increased from 15% to 83% in the atmosphere over Beijing. Unexpectedly, the secondary inorganic fraction in PM2.5 increased with an increase in the ambient RH, which is a meteorological parameter independent of anthropogenic activities, indicating the presence of a feedback mechanism driven by Henry's law and thermodynamic equilibrium. During haze episodes, simultaneously elevated RH levels and anthropogenic secondary inorganic mass concentrations resulted in an abundant ALWC. The condensed water could act as an efficient medium for multiphase reactions, thereby facilitating the transformation of reactive gaseous pollutants into particles and accelerating the formation of heavy haze. ALWC was well correlated with the mass concentrations of both nitrate and sulfate, indicating both nitrate and sulfate salts play key roles in determining ALWC. Coincident with a significant reduction in SO2 emissions throughout China, nitrates will become a dominant anthropogenic inorganic salt driving ALWC. Thus, the abundance of ALWC and its effects on the aerosol chemistry and climate should be reconsidered.
An intensive field campaign was conducted in Chongqing during the summer of 2015 to explore the formation mechanisms of ozone pollution. The sources of ozone, the local production rates, and the controlling factors, as well as key species of volatile organic compounds (VOCs), were quantified by integrating a local ozone budget analysis, calculations of the relative incremental reactivity, and an empirical kinetic model approach. It was found that the potential for rapid local ozone formation exists in Chongqing. During ozone pollution episodes, the ozone production rates were found to be high at the upwind station Nan Quan, the urban station Chao Zhan, and the downwind station Jin-Yun Shan. The average local ozone production rate was 30x10(-9) V/V h(-1) and the daily integration of the produced ozone was greater than 180x10(-9) V/V. High ozone concentrations were associated with urban and downwind air masses. At most sites, the local ozone production was VOC-limited and the key species were aromatics and alkene, which originated mainly from vehicles and solvent usage. In addition, the air masses at the northwestern rural sites were NO (x) -limited and the local ozone production rates were significantly higher during the pollution episodes due to the increased NO (x) concentrations. In summary, the ozone abatement strategies of Chongqing should be focused on the mitigation of VOCs. Nevertheless, a reduction in NO (x) is also beneficial for reducing the regional ozone peak values in Chongqing and the surrounding areas.
Dinitrogen pentoxide (N2O5) is one of the basic trace gases which plays a key role in nighttime atmosphere. An intercomparison and validation of different N2O5 measurement methods is important for determining the true accuracy of these methods. Cavity ring down spectroscopy (CRDS) and cavity enhanced absorption spectrometer (CEAS) were used to measure N2O5 at the campus of the University of Chinese Academy of Sciences (UCAS) from February 21, 2016 to March 4, 2016. The detection limits were 1.6 ppt (1 sigma) at 30 s intervals for the CEAS instrument and 3.9 ppt (1 sigma) at 10 s time resolution for the CRDS instrument respectively. In this study, a comparison of the 1 min observations from the two instruments was presented. The two data sets showed a good agreement within their uncertainties, with an absolute shift of 15.6 ppt, slope of 0.94 and a correlation coefficient R-2 = 0.97. In general, the difference between the CRDS and CEAS instruments for N2O5 measurement can be explained by their combined measurement uncertainties. However, high relative humidity (> 60%) and high PM2.5 concentration (> 200 mu g/m(3)) may contribute to the discrepancies. The excellent agreement between the measurement by the CRDS and CEAS instruments demonstrates the capability of the two instruments for accurately measuring N2O5 with high sensitivity. (C) 2017 Elsevier B.V. All rights reserved.