pH is an important property of aerosol particles but is difficult to measure directly. Several studies have estimated the pH values for fine particles in North China winter haze using thermodynamic models (i.e., E-AIM and ISORROPIA) and ambient measurements. The reported pH values differ widely, ranging from close to 0 (highly acidic) to as high as 7 (neutral). In order to understand the reason for this discrepancy, we calculated pH values using these models with different assumptions with regard to model inputs and particle phase states. We find that the large discrepancy is due primarily to differences in the model assumptions adopted in previous studies. Calculations using only aerosol phase composition as inputs (i.e., reverse mode) are sensitive to the measurement errors of ionic species and inferred pH values exhibit a bimodal distribution with peaks between −2 and 2 and between 7 and 10. Calculations using total (gas plus aerosol phase) measurements as inputs (i.e., forward mode) are affected much less by the measurement errors, and results are thus superior to those obtained from the reverse mode calculations. Forward mode calculations in this and previous studies collectively indicate a moderately acidic condition (pH from about 4 to about 5) for fine particles in North China winter haze, indicating further that ammonia plays an important role in determining this property. The differences in pH predicted by the forward mode E-AIM and ISORROPIA calculations may be attributed mainly to differences in estimates of activity coefficients for hydrogen ions. The phase state assumed, which can be either stable (solid plus liquid) or metastable (only liquid), does not significantly impact pH predictions of ISORROPIA.
Emissions of air pollutants in East Asia play an important role in the regional and global atmospheric environment. In this study we evaluated the recent emission trends of sulfur dioxide (SO2), nitrogen oxides (NOx), particulate matter (PM), and non-methane volatile organic compounds (NMVOC) in East Asia, and projected their future emissions up until 2030 with six emission scenarios. The results will provide future emission projections for the modeling community of the model inter-comparison program for Asia (MICS-Asia). During 2005–2010, the emissions of SO2 and PM2.5 in East Asia decreased by 15 and 12%, respectively, mainly attributable to the large-scale deployment of flue gas desulfurization (FGD) at China's power plants, and the promotion of highly efficient PM removal technologies in China's power plants and cement industry. During this period, the emissions of NOx and NMVOC increased by 25 and 15%, driven by rapid increase in the emissions from China due to inadequate control strategies. In contrast, the NOx and NMVOC emissions in East Asia except China decreased by 13–17%, mainly due to the implementation of stringent vehicle emission standards in Japan and South Korea. Under current regulations and current levels of implementation, NOx, SO2, and NMVOC emissions in East Asia are projected to increase by about one-quarter over 2010 levels by 2030, while PM2.5 emissions are expected to decrease by 7%. Assuming enforcement of new energy-saving policies, emissions of NOx, SO2, PM2.5 and NMVOC in East Asia are expected to decrease by 28, 36, 28, and 15%, respectively, compared with the baseline case. The implementation of "progressive" end-of-pipe control measures would lead to another one-third reduction of the baseline emissions of NOx, and about one-quarter reduction of SO2, PM2.5, and NMVOC. Assuming the full application of technically feasible energy-saving policies and end-of-pipe control technologies, the emissions of NOx, SO2, and PM2.5 in East Asia would account for only about one-quarter, and NMVOC for one-third, of the levels of the baseline projection. Compared with previous projections, this study projects larger reductions in NOx and SO2 emissions by considering aggressive governmental plans and standards scheduled to be implemented in the next decade, and quantifies the significant effects of detailed progressive control measures on NMVOC emissions up until 2030.
China is the largest atmospheric mercury (Hg) emitter in the world. Its Hg emissions and environmental impacts need to be evaluated. In this study, China's Hg emission inventory is updated to 2007 and applied in the GEOS-Chem model to simulate the Hg concentrations and depositions in China. Results indicate that simulations agree well with observed background Hg concentrations. The anthropogenic sources contributed 35–50% of THg concentration and 50–70% of total deposition in polluted regions. Sensitivity analysis was performed to assess the impacts of mercury emissions from power plants, non-ferrous metal smelters and cement plants. It is found that power plants are the most important emission sources in the North China, the Yangtze River Delta (YRD) and the Pearl River Delta (PRD) while the contribution of non-ferrous metal smelters is most significant in the Southwest China. The impacts of cement plants are significant in the YRD, PRD and Central China.