We present a new chemical mechanism for Hg0/HgI/HgII atmospheric cycling, including recent laboratory and computational data, and implement it in the GEOS-Chem global atmospheric chemistry model for comparison to observations. Our mechanism includes the oxidation of Hg0 by Br and OH, subsequent oxidation of HgI by ozone and radicals, respeciation of HgII in aerosols and cloud droplets, and speciated HgII photolysis in the gas and aqueous phases. The tropospheric Hg lifetime against deposition in the model is 5.5 months, consistent with observational constraints. The model reproduces the observed global surface Hg0 concentrations and HgII wet deposition fluxes. Br and OH make comparable contributions to global net oxidation of Hg0 to HgII. Ozone is the principal HgI oxidant, enabling the efficient oxidation of Hg0 to HgII by OH. BrHgIIOH and HgII(OH)2, the initial HgII products of Hg0 oxidation, respeciate in aerosols and clouds to organic and inorganic complexes, and volatilize to photostable forms. Reduction of HgII to Hg0 takes place largely through photolysis of aqueous HgII–organic complexes. 71% of model HgII deposition is to the oceans. Major uncertainties for atmospheric Hg chemistry modeling include Br concentrations, stability and reactions of HgI, and speciation and photoreduction of HgII in aerosols and clouds.
Ozone (O) pollution is becoming increasingly severe in China. In addition, our limited understanding of the relationship between O and volatile organic compounds (VOCs), is an obstacle to improving air quality. By developing an improved source-oriented speciated VOC emission inventory in 2013, we estimated the ozone formation potential (OFP) and investigated its characteristics in China. Besides, a comparison was made between our estimates and space-based observations from the ozone monitoring instrument (OMI) on the National Aeronautics and Space Administration (NASA)'s Aura satellite. According to our estimates, m-/p-xylene, ethylene, formaldehyde, toluene, and propene were the five species that had the largest potential to form ozone, and on-road vehicles, industrial processes, biofuel combustion, and surface coating were the key contributing sectors. Among different regions of China, the North China Plain, Yangtze River Delta, and Pearl River Delta had the highest OFP values. Our results suggest that O formation is VOC-limited in major urban areas of China. Additionally, considering the different photochemical reactivities of various VOC species and the disparate energy and industry structures in the different regions of China, more efficient OFP-based and localized VOC control measures should be implemented, instead of the current mass-based and nationally uniform policies.
Migrant female sex workers (FSWs) are one of the most at-risk populations for HIV in China. This study demonstrates how multiple risk factors are situated and vary by types of sex work environments in a sample of 348 migrant FSWs in Beijing. Participants reported high rates of clients' refusal to use condoms (76%), unsafe sex with both clients (32%), non-paid regular partners (e.g., boyfriend or husband) (76%), and a STI symptom (79%) last year. Only 22% of FSWs had been tested for HIV. Risk factors were compared by three types of sex work environments: (1) entertainment establishments, (2) personal services sectors, and (3) street-based venues, including roadside brothels. Street-based FSWs, compared to the other FSWs, were more likely to be older, married with children, migrate from rural areas, and be arrested by police, and less likely to be educated, have contact with prevention services, be knowledgeable about HIV, and be tested for HIV. The FSWs in entertainment establishments were more likely than streetbased FSWs to have reported being physically, verbally, and/or sexually abused by clients. Multiple discriminant analysis distinguished a profile of two different groups of risk factors: (1) police arrest, lack of protection from violence, access to prevention and health care, and HIV knowledge, and (2) verbal and physical abuse and clients' refusal of condom use. In the massive internal migration in China, disadvantages in economic sectors drive women to become involved in sex work. HIV prevention strategies must target socio-structural factors embedded in sex work environments. Keywordsmigrants; female sex workers; sex work environment; China; HIV preventionChina's open door policy in 1978 toward market-driven economic development led to massive migration from rural to urban areas. In Beijing, an estimated 5.4 million of the 17.4 million city residents in 2007 were migrants (Juan, 2007). Large-scale urbanization also resulted in the reemergence of the sex work industry and a resurgence of sexually transmitted infections (STIs) (Chen et al., 2007;Gil et al, 1996). There are an estimated 10 million FSWs in China (Yang et al., 2005c) As sexual transmission is currently the primary driver of the HIV epidemic in China, the potential spread of HIV via the expanded sexual networks among migrant "floating" populations along with urbanization is of particular concern (Anderson et al., 2003;Yang et al., 2005c). In Li and colleagues' study (2004) of migrants in Beijing, mobility, assessed by the total years of migration and the number of migratory cities, was highly correlated with sexual risk. There have been consistent findings that female migrants reported higher STI rates than male migrants in China (Detels et al., 2003;Liu et al., 2005;Mao & Sun, 1999;Sun, 1997). One of the reasons for this disparity may be women's relative disadvantage to men in socio-economic status, facilitating women's entry into the sex work industry and exposure to other health risks (Huang, 2001;Ren, 1999;Yang & Xia, 2006). Whi...
Abstract. Ambient volatile organic compounds (VOCs) were measured using an online system, gas chromatography–mass spectrometry/flame ionization detector (GC-MS/FID), in Beijing, China, before, during, and after Asia-Pacific Economic Cooperation (APEC) China 2014, when stringent air quality control measures were implemented. Positive matrix factorization (PMF) was applied to identify the major VOC contributing sources and their temporal variations. The secondary organic aerosols potential (SOAP) approach was used to estimate variations of precursor source contributions to SOA formation. The average VOC mixing ratios during the three periods were 86.17, 48.28, and 72.97 ppbv, respectively. The mixing ratios of total VOC during the control period were reduced by 44 %, and the mixing ratios of acetonitrile, halocarbons, oxygenated VOCs (OVOCs), aromatics, acetylene, alkanes, and alkenes decreased by approximately 65, 62, 54, 53, 37, 36, and 23 %, respectively. The mixing ratios of all measured VOC species decreased during control, and the most affected species were chlorinated VOCs (chloroethane, 1,1-dichloroethylene, chlorobenzene). PMF analysis indicated eight major sources of ambient VOCs, and emissions from target control sources were clearly reduced during the control period. Compared with the values before control, contributions of vehicular exhaust were most reduced, followed by industrial manufacturing and solvent utilization. Reductions of these three sources were responsible for 50, 26, and 16 % of the reductions in ambient VOCs. Contributions of evaporated or liquid gasoline and industrial chemical feedstock were slightly reduced, and contributions of secondary and long-lived species were relatively stable. Due to central heating, emissions from fuel combustion kept on increasing during the whole campaign; because of weak control of liquid petroleum gas (LPG), the highest emissions of LPG occurred in the control period. Vehicle-related sources were the most important precursor sources likely responsible for the reduction in SOA formation during this campaign.
Abstract. Isoprene oxidation by nitrate radical (NO3) is a potentially important source of secondary organic aerosol (SOA). It is suggested that the second or later-generation products are the more substantial contributors to SOA. However, there are few studies investigating the multi-generation chemistry of isoprene-NO3 reaction, and information about the volatility of different isoprene nitrates, which is essential to evaluate their potential to form SOA and determine their atmospheric fate, is rare. In this work, we studied the reaction between isoprene and NO3 in the SAPHIR chamber (Jülich) under near-atmospheric conditions. Various oxidation products were measured by a high-resolution time-of-flight chemical ionization mass spectrometer using Br− as the reagent ion. Most of the products detected are organic nitrates, and they are grouped into monomers (C4 and C5 products) and dimers (C10 products) with 1–3 nitrate groups according to their chemical composition. Most of the observed products match expected termination products observed in previous studies, but some compounds such as monomers and dimers with three nitrogen atoms were rarely reported in the literature as gas-phase products from isoprene oxidation by NO3. Possible formation mechanisms for these compounds are proposed. The multi-generation chemistry of isoprene and NO3 is characterized by taking advantage of the time behavior of different products. In addition, the vapor pressures of diverse isoprene nitrates are calculated by different parametrization methods. An estimation of the vapor pressure is also derived from their condensation behavior. According to our results, isoprene monomers belong to intermediate-volatility or semi-volatile organic compounds and thus have little effect on SOA formation. In contrast, the dimers are expected to have low or extremely low volatility, indicating that they are potentially substantial contributors to SOA. However, the monomers constitute 80 % of the total explained signals on average, while the dimers contribute less than 2 %, suggesting that the contribution of isoprene NO3 oxidation to SOA by condensation should be low under atmospheric conditions. We expect a SOA mass yield of about 5 % from the wall-loss- and dilution-corrected mass concentrations, assuming that all of the isoprene dimers in the low- or extremely low-volatility organic compound (LVOC or ELVOC) range will condense completely.
Fine particulate matter (PM), largely composed of secondary organic aerosol (SOA), is currently one of the most intractable environmental problems in China. As crucial precursors for SOA, understanding the formation propensity of various volatile organic compound (VOC) species and sources is useful for pollution control. In this work, we estimated the SOA formation potential (SOAP) of anthropogenic VOC emissions based on an improved speciated VOC emission inventory and investigated its distribution in China. According to our estimates, toluene had the largest SOAP, followed by n-dodecane, m-/p-xylene, styrene, n-decane, and n-undecane, while passenger cars, chemical fiber manufacturing, asphalt paving, and building coating were the top five SOAP-contributing sources nationwide. The spatial distribution of SOAP in China shows a distinct pattern of high values in the southeast and low values in the northwest. Beijing-Tianjin-Hebei and surroundings, the Yangtze River Delta, Pearl River Delta, and Sichuan-Chongqing District were found to have the highest SOAP, particularly in urban areas. The major SOAP-contributing species and sources differed among these regions, which was attributed to local industrial and energy structures. Our results suggest that to mitigate PM pollution in China, more efficient SOAP-based control measures should be implemented instead of current emissions-based policies, and VOC control strategies should be adapted to local conditions.
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