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Screening the emission sources of volatile organic compounds （VOCs） in China by multi-effects evaluation

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Frontiers of Environmental Science & Engineering 2016年第5期10卷 25-35页

作者： He NIU Ziwei MO Min SHAO sihua lu ShaodongXIE State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental Science and Engineering Peking University Beijing 100871 China

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.

关键词： Ozone formation Secondary organic aerosol Multi-effects evaluation VOC abatement strategy

Dissociation of CO on Oxygen Contaminated Ni{001}c(2×2)-Al Surface at Room Temperature

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Chinese Physics Letters 1991年第1期8卷 17-20页

作者： YAO Jun ZHU Li lu sihua WU Sicheng Synchrotron Radiation Laboratoryf Institute of High Energy Physics Academia SinicaBeijing 100039 Department of Physics Zhejiang UniversityHangzhou 310027 Department of PhysicSj Peking University Beijing 100871 Laboratory For Surface Physics Academia SinicaBeijing 100080

The dissociation of CO on oxygen contaminated Ni{001}c(2×2)-Al surface at room temperature has been observed by electron energy loss *** CO dissociation rate is proportional to the oxygen contamination on the surface.

关键词： spectroscopy. surface. dissociation

Reactivity of ambient volatile organic compounds(VOCs) in summer of 2004 in Beijing

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Chinese Chemical Letters 2008年第5期19卷 573-576页

作者： Shan Huang Min Shao sihua lu Ying Liu State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing 100871 China

Ambient volatile organic compounds （VOCs） were sampled at six sites in Beijing in the summer of 2004 and analyzed by GCMS. The chemical reactivities of 73 quantified VOCs species were evaluated by OH loss rates （LOH） and ozone formation potentials （OFPs）. Top 15 reactive species, mainly alkenes and aromatics, were identified by these two methods, and accounted for more than 70% of total reactivity of VOCs. In urban areas, isoprene was the most reactive species in term of OH loss rate, contributing 11.4% to the LOH of VOCs. While toluene, accounting for 9.4% of OFPs, appeared to have a long-time role in the photochemical processes. Tongzhou site is obviously influenced by local chemical industry, but the other five sites showed typical urban features influenced mainly by vehicular emissions.

关键词： VOC Reactivity OH loss rate Ozone formation potential

Investigation of carbonyl compound sources at a rural site in the Yangtze River Delta region of China

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Journal of Environmental Sciences 2015年第2期27卷 128-136页

作者： Ming Wang Wentai Chen Min Shao sihua lu Limin Zeng Min Hu State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking University

Carbonyl compounds are important intermediates in atmospheric photochemistry, but their primary sources are still not understood well. In this work, carbonyls, hydrocarbons,and alkyl nitrates were continuously measured during November 2011 at a rural site in the Yangtze River Delta region of China. Mixing ratios of carbonyls and hydrocarbons showed large fluctuations during the entire measurement. The average level for total measured volatile organic compounds during the pollution episode from 25 th to 27 th November, 2011 was 91.6 ppb, about 7 times the value for the clean period of 7th–8th, November, 2011. To preliminarily identify toluene sources at this site, the emission ratio of toluene to benzene（T/B） during the pollution episode was determined based on photochemical ages derived from the relationship of alkyl nitrates to their parent alkanes. The calculated T/B was5.8 ppb/ppb, significantly higher than the values of 0.2–1.7 ppb/ppb for vehicular exhaust and other combustion sources, indicating the dominant influence of industrial emissions on ambient toluene. The contributions of industrial sources to ambient carbonyls were then calculated using a multiple linear regression fit model that used toluene and alkyl nitrates as respective tracers for industrial emission and secondary production. During the pollution episode, 18.5%, 69.0%, and 52.9% of measured formaldehyde, acetaldehyde, and acetone were considered to be attributable to industrial emissions. The emission ratios relative to toluene for formaldehyde, acetaldehyde, and acetone were determined to be 0.10, 0.20 and0.40 ppb/ppb, respectively. More research on industrial carbonyl emission characteristics is needed to understand carbonyl sources better.

关键词： Carbonyl compounds Source apportionment Industrial emission Yangtze River Delta

Emission factors of gaseous carbonaceous species from residential combustion of coal and crop residue briquettes

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Frontiers of Environmental Science & Engineering 2013年第1期7卷 66-76页

作者： Qin WANG Chunmei GENG sihua lu Wentai CHEN Min SHAO State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing 100871 China Chinese Research Academy of Environmental Sciences Beijing 100012 China

Experiments were performed to measure the emission factors ( s) of gaseous carbonaceous species, such as CO , CO, CH , and non-methane volatile organic compounds (NMVOCs), from the combustion of five types of coal of varying organic maturity and two types of biomass briquettes under residential burning conditions. Samples were collected in stainless steel canisters and 2,4-dinitrophenylhydrazine (DNPH) cartridges and were analyzed by GC–FID/MS and HPLC, respectively. The s from crop residue briquette burning were generally higher than those from coals, with the exception of CO . The dominant NMVOC species identified in coal smoke were carbonyls (41.7%), followed by C2 unsaturated hydrocarbons (29.1%) and aromatics (12.1%), while C2 unsaturated hydrocarbons were the dominant species (68.9%) emitted from the combustion of crop residue briquettes, followed by aromatics (14.4%). A comparison of burning normal crop residues in stoves and the open field indicated that briquettes emitted a larger proportion of ethene and acetylene. Both combustion efficiency and coal organic maturity had a significant impact on NMVOC s from burning coal: NMVOC emissions increased with increasing coal organic maturity but decreased as the combustion efficiency improved. Emissions from the combustion of crop residue briquettes from stoves occurred mainly during the smoldering process, with low combustion efficiency. Therefore, an improved stove design to allow higher combustion efficiency would be beneficial for reducing emissions of carbonaceous air pollutants.

关键词： residential combustion coal crop residue briquette emission factors gaseous carbonaceous species

Major reactive species of ambient volatile organic compounds (VOCs) and their sources in Beijing

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Science China Earth Sciences 2005年第Z2期48卷 147-154页

作者： SHAO Min FU Linlin LIU Ying lu sihua ZHANG Yuanhang TANG Xiaoyan State Joint Key Laboratory of Environmental Simulation and Pollution Control College of Environmental SciencesPeking UniversityBeijing 100871China

Volatile organic compounds(VOCs)are important precursors of atmospheric chemical *** a whole mixture,the ambient VOCs show very strong chemical *** on OH radical loss rates in the air,the chemical reactivity of VOCs in Beijing was *** results revealed that alkenes,accounting for only about 15%in the mixing ratio of VOCs,provide nearly 75%of the reactivity of ambient VOCs and the C4 to C5 alkenes were the major reactive species among the *** study of emission characteristics of various VOCs sources indicated that these alkenes are mainly from vehicle exhaust and gasoline *** reduction of alkene species in these two sources will be effective in photochemical pollution control in Beijing.

关键词： alkenes radicals vehicle exhaust gasoline evaporation.

Chemical speciation and anthropogenic sources of ambient volatile organic compounds (VOCs) during summer in Beijing, 2004

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Frontiers of Environmental Science & Engineering 2007年第2期1卷 147-152页

作者： lu sihua LIU Ying SHAO Min HUANG Shan State Joint Key Laboratory of Environmental Simulation and Pollution Control Peking UniversityBeijing 100871China

Volatile organic compounds(VOCs)were measured at six sites in Beijing in August,*** to 148 VOC species,including C_(3) to C_(12) alkanes,C_(3) to C_(11) alkenes,C_(6) to C_(12) aromatics,and halogenated hydrocarbons,were *** the concentrations differed at the sites,the chemical compositions were similar,except for the Tongzhou site where aromatics were significantly high in the *** on the source profiles measured from previous studies,the source apportionment of ambient VOCs was preformed by deploying the chemical mass balance(CMB)*** results show that urban VOCs are predominant from mobile source emissions,which contribute more than 50% of the VOCs(in mass concentrations)to ambient air at most *** important sources are gasoline evaporation,painting,and *** exception is at the Tongzhou site where vehicle exhaust,painting,and solvents have about equal contribution,around 35% of the ambient VOC *** the receptor model is not valid for deriving the sources of reactive species,such as isoprene and 1,3-butadiene,other methodologies need to be further explored.

关键词： volatile organic compounds(VOCs) chemical composition chemical mass balance model reactive species

Carbonyl emissions from heavy-duty diesel vehicle exhaust in China and the contribution to ozone formation potential

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Journal of Environmental Sciences 2014年第1期26卷 122-128页

作者： Dong Dong Min Shao Yue Li sihua lu Yanjun Wang Zhe Ji Dagang Tang State Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Chinese Research Academy of Environmental Sciences

Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4- dinitrophenyhydrazine cartridge and 23 carbonyl compounds were analyzed by high performance liquid chromatography. The average emission factor of carbonyls was 97.2 mg/km, higher than that of light-duty diesel vehicles and gasoline-powered vehicles. Formaldehyde, acetaldehyde, acetone and propionaidehyde were the species with the highest emission factors. Main influencing factors for carbonyl emissions were vehicle type, average speed and regulated emission standard, and the impact of vehicle loading was not evident in this study. National emission of carbonyls from diesel vehicles exhaust was calculated for China, 2011, based on both vehicle miles traveled and fuel consumption. Carbonyl emission of diesel vehicle was estimated to be 45.8 Gg, and was comparable to gasolinepowered vehicles （58.4 Gg）. The emissions of formaldehyde, acetaldehyde and acetone were 12.6, 6.9, 3.8 Gg, respectively. The ozone formation potential of carbonyls from diesel vehicles exhaust was 537 mg O3/km, higher than 497 mg O3/km of none-methane hydrocarbons emitted from diesel vehicles.

关键词： carbonyl diesel vehicle chassis dynamometer ozone formation potential

Explicit diagnosis of the local ozone production rate and the ozone-NOx-VOC sensitivities

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Science Bulletin 2018年第16期63卷 1067-1076页

作者： Zhaofeng Tan Keding lu Huabin Dong Min Hu Xin Li Yuhan Liu sihua lu Min Shao Rong Su Haichao Wang Yusheng Wu Andreas Wahner Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University. Beijing 100871 China Institute of Energy and Climate Research IEK-8: Troposphere Forschungszentrum julich GmbH Julich 52428 Germany Beijing Innovation Center for Engineering Sciences and Advanced Technology Peking University Beijing 100871 China

In the troposphere, ozone is a harmful gas compound to both human health and vegetation. Ozone is produced from the reaction of NO_x(@NO + NO_2) and VOCs(volatile organic compounds) with light. Due to the highly nonlinear relationships between ozone and its precursors, proper ozone mitigation relies on the knowledge of chemical mechanisms. In this study, an observation-based method is used to simulate ozone formation and elucidate its controlling factors for a rural site on the North China Plain. The instantaneous ozone production rate is calculated utilizing a box model using the dataset obtained from the Wangdu campaign. First, the model was operated in a time-dependent mode to calculate the ozone production rate at each time stamp. The calculated ozone formation rate showed a diurnal average maximum value of 17 ppbv/h(1-h diurnal averaged). The contribution of individual peroxy radicals to ozone production was analyzed. In addition, the functional dependence of calculated P(O_3) reveals that ozone production was in a NO_x-limited regime during the campaign. Furthermore, the missing peroxy radical source will further extend NO_x-limited conditions to earlier in the day, making NO_xlimitation dominate more of a day than the current chemical model predicts. Finally, a multiple scenarios mode,also known as EKMA(empirical kinetic modeling approach), was used to simulate the response of P(O_3) to the imaginary change in precursor concentrations. We found that ozone production was in the NO_x-limited region. However, the use of NO_2 measured by the molybdenum converter and/or the absence of a peroxy radical source in the current chemical model could over-emphasize the VOC-limited effect on ozone production.

关键词： Observational-based model Instantaneous ozone production rate (empirical kinetic modeling approach) EKMA