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Aqueous-phase formation of N-containing secondary organic compounds affected by the ionic strength

Journal of environmental Sciences 2024年第4期138卷 88-101页

作者： Yuqi Gan Xiaohui Lu Shaodong Chen Xinghua Jiang Shanye Yang Xiewen Ma Mei Li Fan Yang Yewen Shi Xiaofei Wang Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science and EngineeringFudan UniversityShanghai 200433China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Guangdong Provincial Observation and Research station for Coastal Atmosphere and Climate of the Great Bay Area Southern University of Science and TechnologyShenzhen 518055China Institute of Mass Spectrometry and Atmospheric Environment Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air PollutionJinan UniversityGuangzhouChina environmental monitoring station of pudong new district Shanghai 201200China Shanghai Municipal Center for Disease Control&Prevention Shanghai 200336China

The reaction of carbonyl-to-imine/hemiaminal conversion in the atmospheric aqueous phase is a critical pathway to produce the light-absorbing N-containing secondary organic compounds(SOC).The formation mechanism of these compounds has been wildly investigated in bulk solutions with a low ionic strength.However,the ionic strength in the aqueous phase of the polluted atmosphere may be higher.It is still unclear whether and to what extent the inorganic ions can affect the SOC formation.Here we prepared the bulk solution with certain ionic strength,in which glyoxal and ammonium were mixed to mimic the aqueous-phase reaction.Molecular characterization by High-resolution Mass Spectrometry was performed to identify the N-containing products,and the light absorption of the mixtures was measured by ultraviolet-visible spectroscopy.Thirty-nine N-containing compounds were identified and divided into four categories(N-heterocyclic chromophores,high-molecular-weight compounds with N-heterocycle,aliphatic imines/hemiaminals,and the unclassified).It was observed that the longer reaction time and higher ionic strength led to the formation of more N-heterocyclic chromophores and the increasing of the lightabsorbance of the mixture.The added inorganic ions were proposed to make the aqueous phase somewhat viscous so that the molecules were prone to undergo consecutive and intramolecular reactions to form the heterocycles.In general,this study revealed that the enhanced ionic strength and prolonged reaction time had the promotion effect on the lightabsorbing SOC formation.It implies that the aldehyde-derived aqueous-phase SOC would contribute more light-absorbing particulate matter in the industrial or populated area where inorganic ions are abundant.

关键词： Ionic strength Carbonyl-to-imine/hemiaminal Heterocyclic Brown carbon Mass spectrometry Aqueous-phase reaction

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Mixing states and secondary formation processes of organic nitrogen-containing single particles in Guangzhou,China

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Journal of environmental Sciences 2024年第4期138卷 62-73页

作者： Lijun Yun Chunlei Cheng Suxia Yang Zaihua Wang Mei Li Qi En Zhong LiyuanMao Sulin Liu Xiaoya Cheng Duanying Chen Fan Yang Zhen Zhou Institute of Mass Spectrometry and Atmospheric Environment Guangdong Provincial Engineering Research Center for on-line source apportionment system of air pollutionJinan UniversityGuangzhou 510632China Guangdong-Hongkong-Macao Joint Laboratory of Collaborative Innovation for environmental Quality Guangzhou 510632China State Key Laboratory of Loess and Quaternary Geology Institute of Earth EnvironmentChinese Academy ScienceXi’an 710061China Institute for Environment and Climate Research Jinan UniversityGuangzhou 510632China Guangdong Academy of Sciences Institute of Resources Utilization and Rare Earth DevelopmentGuangzhou 510650China environmental monitoring station of pudong new district Shanghai 201200China

Organic nitrogen(ON)compounds play a significant role in the light absorption of brown carbon and the formation of organic aerosols,however,the mixing state,secondary formation processes,and influencing factors of ON compounds are still unclear.This paper reports on the mixing state of ON-containing particles based on measurements obtained using a highperformance single particle aerosol mass spectrometer in January 2020 in Guangzhou.The ON-containing particles accounted for 21% of the total detected single particles,and the particle count and number fraction of the ON-containing particles were two times higher at night than during the day.The prominent increase in the content of ON-containing particles with the enhancement of NO_xmainly occurred at night,and accompanied by high relative humidity and nitrate,which were associated with heterogeneous reactions between organics and gaseous NO_(x)and/or NO_(3)radical.The synchronous decreases in ON-containing particles and the mass absorption coefficient of water-soluble extracts at 365 nm in the afternoon may be associated with photo-bleaching of the ON species in the particles.In addition,the positive matrix factorization analysis found five factors dominated the formation processes of ON particles,and the nitrate factor(33%)mainly contributed to the production of ON particles at night.The results of this study provide unique insights into the mixing states and secondary formation processes of the ON-containing particles.

关键词： Organic nitrogen compounds Single particles Mixing state Secondary formation Nighttime chemistry

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Response of PM_(2.5)-bound elemental species to emission variations and associated health risk assessment during the COVID-19 pandemic in a coastal megacity

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Journal of environmental Sciences 2022年第12期34卷 115-127页

作者： Guochen Wang Kan Huang Qingyan Fu Jia Chen Juntao Huo Qianbiao Zhao Yusen Duan Yanfen Lin Fan Yang Wenjie Zhang Hao Li Jian Xu Xiaofei Qin Na Zhao Congrui Deng Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Department of Environmental Science and EngineeringFudan UniversityShanghai 200433China Shanghai environmental monitoring Center Shanghai 200030China pudong new district environmental monitoring station Shanghai 200122China Chinese Research Academy of environmental Sciences Beijing 100012China IRDR ICoE on Risk Interconnectivity and Governance on Weather/Climate Extremes Impact and Public Health Fudan UniversityShanghai 200433China Institute of Eco-Chongming(IEC) Shanghai 202162China

The coronavirus(COVID-19)pandemic is disrupting the world from many aspects.In this study,the impact of emission variations on PM_(2.5)-bound elemental species and health risks associated to inhalation exposure has been analyzed based on real-time measurements at a remote coastal site in Shanghai during the pandemic.Most trace elemental species decreased significantly and displayed almost no diel peaks during the lockdown.After the lockdown,they rebounded rapidly,of which V and Ni even exceeded the levels before the lockdown,suggesting the recovery of both inland and shipping activities.Five sources were identified based on receptor modeling.Coal combustion accounted for more than 70%of the measured elemental concentrations before and during the lockdown.Shipping emissions,fugitive/mineral dust,and waste incineration all showed elevated contributions after the lockdown.The total non-carcinogenic risk(HQ)for the target elements exceeded the risk threshold for both children and adults with chloride as the predominant species contributing to HQ.Whereas,the total carcinogenic risk(TR)for adults was above the acceptable level and much higher than that for children.Waste incineration was the largest contributor to HQ,while manufacture processing and coal combustion were the main sources of TR.Lockdown control measures were beneficial for lowering the carcinogenic risk while unexpectedly increased the non-carcinogenic risk.From the perspective of health effects,priorities of control measures should be given to waste incineration,manufacture processing,and coal combustion.A balanced way should be reached between both lowering the levels of air pollutants and their health risks.

关键词： COVID-19 lockdown PM_(2.5)-bound elemental species Source apportionment Health risk Shanghai

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Sorption and cosorption of the nonionic herbicide mefenacet and heavy metals on soil and its components

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Journal of environmental Sciences 2012年第3期24卷 427-434页

作者： Zhenyu Liu Huiqin Guo Huan He Cheng Sun State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210046China Shanghai pudong new Area environmental monitoring station Shanghai 200135China

Sorption and cosorption of the nonionic herbicide mefenacet and two typical metals （copper and silver） on black soil and its components （kaolinite and humic acid） were investigated. It was found that because of their different valences and properties, Cu2＋and Ag＋ presented different effects on the sorption of mefenacet. Due to the competition of Cu2＋, along with the shells of dense water formed by its surface complexation, for sorption surface area with mefenacet, the addition of Cu2＋ decreased the sorption amount of mefenacet on soil and its components, especially on humic acid. However, the addition of Ag＋ significantly enhanced the sorption of mefenacet, which was attributed to the softness of the cation that weakened the hydrophilicity of the local region around Ag＋-complexed functionalities, and thus mitigated the competitive sorption of water. In addition, the sorption of mefenacet on soil with or without the two metals was generally decreased with increasing pH, which was caused by the hydrolysis of carbonyl and carboxyl groups on the surface of the sorbents, π-π interaction between mefenacet and the soil organic matter, and so on. On the other hand, the presence of mefenacet seemed to have little effect on the sorption of Cu2＋ and Ag＋, indicating that Cu2＋ and Ag＋ might be sorbed strongly on the tested sorbents and the mefenacet added was too low in concentration to affect the sorption of the metals.

关键词： mefenacet copper silver soil kaolinite humic acid adsorption pH

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Drip fertigation and plant hedgerows significantly reduce nitrogen and phosphorus losses and maintain high fruit yields in intensive orchards

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Journal of Integrative Agriculture 2023年第2期22卷 598-610页

作者： SONG Ke QIN Qin YANG Ye-feng SUN Li-juan SUN Ya-fei ZHENG Xian-qing Lü Wei-guang XUE Yong Eco-environmental Protection Research Institute Shanghai Academy of Agricultural SciencesShanghai 201403P.R.China pudong new district Agro-Technology Extension Service Center Shanghai 201300P.R.China

A field experiment was carried out to evaluate the effects of drip fertigation combined with plant hedgerows on nitrogen and phosphorus runoff losses in intensive pear orchards in the Tai Lake Basin.Nitrogen and phosphorus runoff over a whole year were measured by using successional runoff water collection devices.The four experimental treatments were conventional fertilization(CK),drip fertigation(DF),conventional fertilization combined with plant hedgerows(C+H),and drip fertigation combined with plant hedgerows(D+H).The results from one year of continuous monitoring showed a significant positive correlation between precipitation and surface runoff discharge.Surface runoff discharge under the treatments without plant hedgerows totaled 15.86%of precipitation,while surface runoff discharge under the treatments with plant hedgerows totaled 12.82%of precipitation.Plant hedgerows reduced the number of runoff events and the amount of surface runoff.Precipitation is the main driving force for the loss of nitrogen and phosphorus in surface runoff,and fertilization is an important factor affecting the losses of nitrogen and phosphorus.In CK,approximately 7.36%of nitrogen and 2.63%of phosphorus from fertilization entered the surface water through runoff.Drip fertigation reduced the accumulation of nitrogen and phosphorus in the surface soil and lowered the runoff loss concentrations of total nitrogen(TN)and total phosphorus(TP).Drip fertigation combined with plant hedgerows significantly reduced the overall TN and TP losses by 45.38 and 36.81%,respectively,in comparison to the CK totals.Drip fertigation increased the vertical migration depth of nitrogen and phosphorus nutrients and reduced the accumulation of nitrogen and phosphorus in the surface soil,which increased the pear yield.The promotion of drip fertigation combined with plant hedgerows will greatly reduce the losses of nitrogen and phosphorus to runoff and maintain the high fruit yields in the intensive orchards of the Tai Lake Basin.

关键词： drip fertigation plant hedgerows surface runoff nitrogen and phosphorus losses fruit yields

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Analysis of VOCs Pollution Characteristics and Ozone Formation Potential Based on a Mobile monitoring System in Beibei district

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Meteorological and environmental Research 2022年第6期13卷 31-34,41页

作者： Xianshuang YANG Ecological Environment monitoring station of Beibei district Chongqing 400700China

Based on a mobile monitoring system,101 volatile organic compounds(VOCs)in ambient air near a national control station in an industrial park were monitored during February 15-21 in 2022,and the pollution characteristics and ozone formation potential(OFP)of VOCs were analyzed.The results show that among the top 10 VOCs with higher mass concentration,there were 5 VOCs appearing in each day from February 15 to 21,including styrene,benzene,toluene,undecane and n-decane,which indicates that the sources of VOCs emission at the monitoring point were relatively stable.During the monitoring period,aromatic hydrocarbons contributed the most to the ozone formation potential of VOCs,accounting for above 70%,followed by alkanes and oxygen-containing compounds.The total OFP of aromatic hydrocarbons,alkanes and oxygen-containing compounds accounted for more than 90%,so they became the active components with the greatest influence on ozone formation.Aromatic hydrocarbons such as 1,2,4-trimethylbenzene,1,3,5-trimethylbenzene and m/p-dimethylbenzene,oxygen-containing organic compounds such as ethanol and acetone,and alkanes such as n-nonane and butane had high OFP,so they had a great effect on ozone formation.

关键词： VOCs Pollution characteristics OFP

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Operating pesticide use reduction within the boundary of food security in peri-urban settings

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Fundamental Research 2022年第4期2卷 635-647页

作者： Yuquan W.Zhang Bruce A.McCarl Zhengwei Cao Qiang Li Shaohua Yang Huiwen Liu China-UK Low Carbon College Shanghai Jiao Tong UniversityNo.3 Yinlian RoadPudong New AreaShanghai 201306China Department of Agricultural Economics Texas A&M University2124 TAMUCollege StationTexas 77843USA School of Agriulureand Biology Shanghai Jiao Tong UniversiyNo.800 Dongchuan RoodMinhang District Shanghai 200240China

Pesticide use in peri-urban areas afects the urban enviroment and public health,and reducing the use may present food security isues for urban dwellers.In this study,we explore how a muiallyadopted goal of a 20%reduetion in pesticide use could be achieved,along with local food security and environmental implica-tions,for Shanghai located in the densely populated East China.A regional Shanghai Agricultural Sector Model inorporating district-and technology-varying crop budgets,was developed to simulate the efects of pesticide reduction policy.Here we find that achieving the reduction goal had the largest implications in districts with high pesticide use totals and intensities,potentially reducing pesticide non point source pollution in the Yangtze River Estuary and Dianshan Lake;the production levels of rice and leafy vegetables would be most afected;and adopting machinery that allows more precise pesticide application modulates these results.Moreover,imposing the requlrements at the district-level caused more severe local food security concerns,and less environmental benefits.Furthermore,a closed Shanghai's agricultural economy would subtantally enlarge the regional het-erogeneity in the above-mentioaned outcomes.Exploring the ffects of a quantity control policy on current-use pesticides at diferent aggregation levels has important implications for regulating the use of agrochemicals.

关键词： Pesticide use reduction Shanghai Agricultural Sector Model(SH-ASM) Peri-urban agriculture Crop budget Cropmix

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Enhanced mixing state of black carbon with nitrate in single particles during haze periods in Zhengzhou, China

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Journal of environmental Sciences 2022年第1期34卷 185-196页

作者： Qianni Zhou Chunlei Cheng Suxia Yang Minghao Yuan Jingjing Meng Haifeng Gong Qien Zhong Yao Zhang Yutong Xie Zhen Zhou Mei Li Institute of Mass Spectrometry and Atmospheric Environment Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air PollutionJinan UniversityGuangzhou 510632China Guangdong-Hongkong-Macao Joint Laboratory of Collaborative Innovation for environmental Quality Guangzhou 510632China School of Environment and Planning Liaocheng UniversityLiaocheng 252000China Institute for Environment and Climate Research Jinan UniversityGuangzhou 510632China Zhengzhou environmental Protection monitoring Center station Zhengzhou 450007China

Black carbon(BC)plays an important role in air quality and climate change,which is closely associated with its mixing state and chemical compositions.In this work the mixing state of BC-containing single particles was investigated to explore the evolution process of ambient BC particles using a single particle aerosol mass spectrometer(SPAMS)in March 2018 in Zhengzhou,China.The BC-containing particles accounted for 61.4%of total detected ambient single particles and were classified into five types including BC-nitrate(BC-N,52.3%)as the most abundant species,followed by BC-nitrate-sulfate(BC-NS,22.4%),BCOC(16.8%),BC-fresh(BC-F,4.5%)and BC-sulfate particles(BC-S,4.0%).With enhancement of the ambient nitrate concentration,the relative peak area(RPA)of nitrate in BC-N and BC–NS particles both increased,yet only the number fraction(N_(f))of BC–N particles increased while the N_(f) of BC-NS particles decreased,suggesting that the enhanced mixing state of BC with nitrate was mainly due to the increase in the ambient nitrate mass concentration.In addition,the Nfof BC-N decreased from 65.3%to 28.4%as the absorbing Angstrom exponents(AAE)of e BC increased from 0.75 to 1.45,which indicated the reduction of light absorption ability of aged BC particles with the enhanced formation of BC-N particles.The results of this work indicated a change in the mixing state of BC particles due to the dominance of nitrate in PM_(2.5),which also influenced the optical properties of aged BC particles.

关键词： Single particle Black carbon Mixing state Nitrate Aging process

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Numerical Simulation of Distribution of VOCs Concentration in the Main Urban Area of Chongqing Based on CALPUFF

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Meteorological and environmental Research 2022年第4期13卷 14-18,24页

作者： Pingjiang LV Zhenliang LI Min CHEN Dan ZHANG Huachun LI Chongqing Academy of Ecological environmental Sciences Chongqing 401147China Southwest Branch of Chinese Research Academy of environmental Sciences Chongqing 401147China Wanzhou district Ecological Environment monitoring station Chongqing 404100China

The distribution of VOCs concentration in the main urban area of Chongqing was simulated based on the CALPUFF model.The results show that the long-term contribution of key industrial pollution sources of VOCs in the study area was not significant(0-0.13 mg/m^(3)),and the hourly average instantaneous contribution was significant(the maximum was up to 2.75 mg/m^(3));the hourly average concentration of VOCs in the area where the sensitive points were located rose abruptly at different times(with a maximum of 1.35 mg/m^(3)).The distribution of VOCs concentration in this area was influenced by the dominant wind,and the area where the sensitive points were located was not the area covered by the maximum landing concentration of pollutants.As the dominant wind changed,the pollution situation of the sensitive points may be worsen.

关键词： CALPUFF model VOCs Spatial distribution Numerical simulation

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WRF Numerical Simulation Analysis of Meteorological Elements in the Main Urban Area of Chongqing from 2013 to 2015

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Meteorological and environmental Research 2022年第4期13卷 59-61,66页

作者： Rui YUAN Zhenliang LI Dan ZHANG Wei HU Huachun LI Chongqing Academy of Ecological environmental Sciences Chongqing 401147China Southwest Branch of Chinese Research Academy of environmental Sciences Chongqing 401147China Wanzhou district Ecological Environment monitoring station Chongqing 404100China

Using the WRF mesoscale numerical model,based on the FNL global reanalysis data of NCEP,numerical simulations with a resolution of 27,9 and 3 km were carried out on the meteorological elements in four national air quality control stations(Jinyun Mountain,Shapingba,Jiefangbei and Nanping)in the main urban area of Chongqing City in July from 2013 to 2015.The results show that at the concerned points,there was an obvious southeast dominant wind at 850 hPa.The meteorological conditions in July in the main urban area of Chongqing were favorable for the diffusion of pollutants.That is,the height of the mixed layer was higher,and the precipitation was higher;the temperature and wind speed at 850 hPa were higher.Compared with 2013 and 2014,the meteorological conditions in July 2015 were not more favorable for the diffusion of pollutants.

关键词： WRF Numerical simulation Meteorological conditions Chongqing City

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