Volatile organic compounds (VOCs) play important roles in the atmosphere via three main pathways: photochemical ozone formation, secondary organic aerosol production, and direct toxicity to humans. Fewstudies have ...Volatile organic compounds (VOCs) play important roles in the atmosphere via three main pathways: photochemical ozone formation, secondary organic aerosol production, and direct toxicity to humans. Fewstudies have integrated these effect, s to prioritize control measures for VOC.s sources. In this study,we developed a multi-effects evaluation methodology based on updated emission inventories and source profiles, by combining the ozone formation potential (OFP), secondary organic aerosol potential (SOAP), and VOC toxicity data. We derived species-specific emission inventories for 152 sources. The OFPs, SOAPs, and toxicity of each source were estimated, the contribution and sharing of source to each of these adverse effects were calculated. Weightings were given to the three adverse effects by expert scoring, and then the integrated effect was determined. Taking 2012 as the base year,solvent use and industrial process were found to be the most important anthropogenic sources, accounting for 24.2% and 23.1% of the integrated effect, respectively, followed by biomass burning, transportation, and fossil fuel combustion, each had a similar contribution ranging from 16.7% to 18.6%. The top five industrial sources, including plastic products, rubber products, chemical fiberproducts, the chemical industry, and oil refining, accounted for nearly 70.0% of industrial emissions. Beijing, Chongqing, Shanghai, Jiangsu, and Guangdong were the five provinces contributing the largest integrated effects. For the VOC species from emissions showed the largest contributions were styrene, toluene, ethylene, benzene, and m/p-xylene.展开更多
Vehicle evaporation is an essential source of VOCs in cities but is not well understood in China.Reported emission factors from previous studies are not enough for understanding the atmospheric chemical process of veh...Vehicle evaporation is an essential source of VOCs in cities but is not well understood in China.Reported emission factors from previous studies are not enough for understanding the atmospheric chemical process of vehicular evaporative VOCs.In this work,a serious of detailed VOCs speciation profiles are developed based on test processes and emission processes.A mass balance method was used to divide different emission processes during diurnal tests.The results show that headspace vapor of gasoline cannot represent the real-world vehicle evaporation because of the significant differences in VOCs speciation profiles,especially for aromatics.To further distinguish emissions from evaporation and exhaust,only the ratios of MTBE/benzene and MTBE/toluene can serve as indicators when considering species from all evaporative processes.Besides,emissions from different sources change significantly with the seasons.To solve these problems,we developed a monthly comprehensive evaporation speciation profile.The individual profiles at the emission processes are weighted by the emission of the in-use vehicle fleet in Beijing to derive the comprehensive speciation profile of evaporative VOCs.Ozone formation potential(OFP)and secondary organic aerosol potential(SOAP)were used to evaluate the environmental impact.For SOAP,100 g evaporative emissions are equal to 6.05-12.71 g toluene in different months,much higher than that given using headspace vapors,especially in winter(7.2 times higher in December).These findings would improve our understanding of the evaporative VOCs emissions in China and their environmental impacts(e.g.,O3 and SOA formation).展开更多
Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds(VOCs). However,little information on secondary aeroso...Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds(VOCs). However,little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4–5 hr simulation, which was estimated to represent more than 10 days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol(SOA) production was 426 ± 85 mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China.展开更多
基金This study was funded by the Natural Science Foundation for Outstanding Young Scholars (Grant No. 41125018) and Natural Science Foundation Key Project (Grant No. 41330635). The fimding source was involved in the data collection of this paper.
文摘Volatile organic compounds (VOCs) play important roles in the atmosphere via three main pathways: photochemical ozone formation, secondary organic aerosol production, and direct toxicity to humans. Fewstudies have integrated these effect, s to prioritize control measures for VOC.s sources. In this study,we developed a multi-effects evaluation methodology based on updated emission inventories and source profiles, by combining the ozone formation potential (OFP), secondary organic aerosol potential (SOAP), and VOC toxicity data. We derived species-specific emission inventories for 152 sources. The OFPs, SOAPs, and toxicity of each source were estimated, the contribution and sharing of source to each of these adverse effects were calculated. Weightings were given to the three adverse effects by expert scoring, and then the integrated effect was determined. Taking 2012 as the base year,solvent use and industrial process were found to be the most important anthropogenic sources, accounting for 24.2% and 23.1% of the integrated effect, respectively, followed by biomass burning, transportation, and fossil fuel combustion, each had a similar contribution ranging from 16.7% to 18.6%. The top five industrial sources, including plastic products, rubber products, chemical fiberproducts, the chemical industry, and oil refining, accounted for nearly 70.0% of industrial emissions. Beijing, Chongqing, Shanghai, Jiangsu, and Guangdong were the five provinces contributing the largest integrated effects. For the VOC species from emissions showed the largest contributions were styrene, toluene, ethylene, benzene, and m/p-xylene.
基金supported by the National Key R&D Program(2016YFC0201504)the National Natural Science Foundation of China(Nos.41822505 and 41571447)+2 种基金National Research Program for Key Issues in Air Pollution Control(DQGG0201&0207)Beijing Nova Program(Z181100006218077)SEE Foundation.
文摘Vehicle evaporation is an essential source of VOCs in cities but is not well understood in China.Reported emission factors from previous studies are not enough for understanding the atmospheric chemical process of vehicular evaporative VOCs.In this work,a serious of detailed VOCs speciation profiles are developed based on test processes and emission processes.A mass balance method was used to divide different emission processes during diurnal tests.The results show that headspace vapor of gasoline cannot represent the real-world vehicle evaporation because of the significant differences in VOCs speciation profiles,especially for aromatics.To further distinguish emissions from evaporation and exhaust,only the ratios of MTBE/benzene and MTBE/toluene can serve as indicators when considering species from all evaporative processes.Besides,emissions from different sources change significantly with the seasons.To solve these problems,we developed a monthly comprehensive evaporation speciation profile.The individual profiles at the emission processes are weighted by the emission of the in-use vehicle fleet in Beijing to derive the comprehensive speciation profile of evaporative VOCs.Ozone formation potential(OFP)and secondary organic aerosol potential(SOAP)were used to evaluate the environmental impact.For SOAP,100 g evaporative emissions are equal to 6.05-12.71 g toluene in different months,much higher than that given using headspace vapors,especially in winter(7.2 times higher in December).These findings would improve our understanding of the evaporative VOCs emissions in China and their environmental impacts(e.g.,O3 and SOA formation).
基金supported by the National Key Basic Research and Development Program (No. 2013CB228500)the National Basic Research Program (973) of China (Nos. 2013CB228503, 2013CB228502)+3 种基金National Natural Science Foundation of China (Nos. 91544214, 51636003)the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB05010500)China Postdoctoral Science Foundation (No. 2015M580929)the State Key Lab of Automotive Safety and Energy at Tsinghua University for their support for the experiments
文摘Light-duty gasoline vehicles have drawn public attention in China due to their significant primary emissions of particulate matter and volatile organic compounds(VOCs). However,little information on secondary aerosol formation from exhaust for Chinese vehicles and fuel conditions is available. In this study, chamber experiments were conducted to quantify the potential of secondary aerosol formation from the exhaust of a port fuel injection gasoline engine. The engine and fuel used are common in the Chinese market, and the fuel satisfies the China V gasoline fuel standard. Substantial secondary aerosol formation was observed during a 4–5 hr simulation, which was estimated to represent more than 10 days of equivalent atmospheric photo-oxidation in Beijing. As a consequence, the extreme case secondary organic aerosol(SOA) production was 426 ± 85 mg/kg-fuel, with high levels of precursors and OH exposure. The low hygroscopicity of the aerosols formed inside the chamber suggests that SOA was the dominant chemical composition. Fourteen percent of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatile organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reductions of emissions of aerosol precursor gases from vehicles are essential to mediate pollution in China.