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Significant contribution of carbonyls to atmospheric oxidation capacity(AOC)during the winter haze pollution over North China Plain

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Journal of Environmental Sciences 2024年第5期139卷 377-388页

作者： Xue Yang Gen Zhang Guang Pan Guolan Fan Houyong Zhang Xuan Ge Mingyue Du School of Municipal and Environmental Engineering Shandong Jianzhu UniversityJi’nan 250101China State Key Laboratory of Severe Weather&Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological SciencesBeijing 100081China Shandong Jinan Ecological Environment Monitoring Center Ji’nan 250101China

Atmospheric carbonyl compounds play significant roles in the cycling of radicals and have exhibited surprisingly high levels in winter that were well correlated to particulate matter,for which the reason have not been clearly *** we measured carbonyl compounds and other trace gasses together with PM_(2.5)over urban Jinan in North China Plain during the *** higher carbonyl concentrations(average:14.63±4.21 ppbv)were found during wintertime haze pollution,about one to three-times relative to those on nonhaze days,with slight difference in chemical composition except formaldehyde(HCHO).HCHO(3.68 ppbv),acetone(3.17 ppbv),and acetaldehyde(CH_3CHO)(2.83 ppbv)were the three most abundant species,accounting for~75% of the total carbonylson both haze and non-haze *** from observational-based model(OBM)with atmospheric oxidation capacity(AOC)indicated that AOC significantly increased with the increasing carbonyls during the winter haze *** photolysis have supplied key oxidants such as RO_(2) and HO_(2),and thereby enhancing the formation of fine particles and secondary organic aerosols,elucidating the observed haze-carbonyls *** variation with carbonyls exhibiting peak values at early-noon and night highlighted the combined contribution of both secondary formation and primary diesel-fuel sources.1-butene was further confirmed to be the major precursor for *** study confirms the great contribution of carbonyls to AOC,and also suggests that reducing the emissions of carbonyls would be an effective way to mitigate haze pollution in urban area of the NCP region.

关键词： Carbonyls haze Observation-based model Source apportionment Atmospheric oxidation capacity

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haze observations by simultaneous lidar and WPS in Beijing before and during APEC, 2014

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Science China Chemistry 2015年第9期58卷 1385-1392页

作者： Zhenyi Chen Jiaoshi Zhang Tianshu Zhang Wenqing Liu Jianguo Liu Anhui Institute of Optics and Fine Mechanics Chinese Academy of Sciences

We present combined Mie lidar, ozone lidar and wide-range particle spectrometer observations which were carried out in Beijing, north China during two periods—one haze period before the Asia-Pacific Economic Cooperation(APEC) meeting and one moderate pollution period during the meeting in 2014. High extinction coefficient, moderate ozone concentration and variable particle number concentration were obtained throughout the first haze observation period. The mean extinction coefficients in the two pollution periods were 0.52 and 0.23 km?1, respectively, at 532 nm. The ozone concentration during the first haze phase was more various with a higher average value of 49 ppb compared with that in the second pollution observations(32 ppb). Compared with the same metrological condition occurring at the end of October, the sharply decreased aerosol extinction coefficient and ozone concentration show the effectiveness of the emission-cutting measures implemented during APEC in November. The comparison of aerosols and ozone in different heights indicate different pollution sources and the complicated ozone process of generation and disappearance. The correlation between the scattering coefficient and particle number concentrations of various diameter depended on the ambient humidity. Especially the particle number concentration(500 nm–1 ?m) contributed most to PM2.5 concentration. The four-day back trajectories from a Hybrid Single-particle Lagrangian Integrated Trajectory(HYSPLIT) model indicate that the air masses in the lower boundary layer before and during APEC were advected from the densely populated south regions of China and the long pollution transportation passing through northern China.

关键词： haze aerosol ozone lidar WPS

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A monitoring-modeling approach to SO_4^(2-) and NO_3^- secondary conversion ratio estimation during haze periods in Beijing, China

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Journal of Environmental Sciences 2019年第4期31卷 293-302页

作者： Xiaoqi Wang Wei Wei Shuiyuan Cheng Chong Zhang Wenjiao Duan Key Laboratory of Beijing on Regional Air Pollution Control Beijing University of Technology Collaborative Innovation Center of Beijing City Traffic Beijing University of Technology

SO_4^(2-) and NO_3^- are important chemical components of fine particulate matter(PM_(2.5)),especially during haze *** study selected two haze episodes in Beijing,China with similar meteorological conditions.A monitoring-modeling approach was developed to estimate the secondary conversion ratios of sulfur and nitrogen based on monitored and simulated *** showed that in Episode 1(24th–25th October,2014),the concentrations(proportions)of SO_4^(2-) and NO_3^- reached 35.1μg/m^3(14.9%) and 55.0μg/m^3(22.9%),while they reached 14.4μg/m^3(9.3%) and 59.1μg/m^3(38.1%)in Episode 2(26th–27th October,2017).A modeling system was applied to apportion Beijing's SO_4^(2-) and NO_3^- in primary and secondary SO_4^(2-)/NO_3^- emitted from local and regional ***,secondary conversion contributions considering the local and regional level were *** former primarily focused on Beijing atmospheric oxidation ability and the latter mainly considered the existence form of Beijing SO_4^(2-)/NO_3^- under the regional transport ***,secondary oxidation ratios were estimated through combining secondary conversion contribution coefficients for simulated and monitored *** regional level,sulfur oxidation ratios in polluted(clean)days during two sampling periods were0.57–0.72(0.07–0.52)and 0.74–0.80(0.08–0.61),nitrogen oxidation ratios were 0.20–0.29(0.05–0.15)and 0.34–0.38(0.02–0.29),indicating that atmospheric oxidation was enhanced when considering regional transport through 2014–*** the local level,sulfur oxidation ratios were 0.66–0.71(0.04–0.48)in haze(clean)days,while nitrogen oxidation ratios were0.16–0.29(0.02–0.16).The atmospheric oxidation ability markedly increased in PM_(2.5)pollution days,but changed only slightly between the two periods.

关键词： haze periods SO42- and NO3- Secondary conversion Secondary oxidation ratio

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Surface active agents stabilize nanodroplets and enhance haze formation

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Chinese Physics B 2021年第1期30卷 94-99页

作者： Yunqing Ma Changsheng Chen Xianren Zhang State Key Laboratory of Organic-inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

Although many organic molecules found commonly in the atmosphere are known to be surface-active in aqueous solutions, their effects on the mechanisms underlying haze formation remain unclear. In this paper, based on a simple thermodynamic analysis, we report that the adsorption of amphiphilic organics alone not only lowers the surface tension,but also unexpectedly stabilizes nanodroplets of specific size under water vapor supersaturation. Then we determine how various factors, including relative humidity, water activity effect due to dissolution of inorganic components as well as surface tension effect due to surface adsorption of organic components, cooperatively induce the stability of *** nanodroplet stability behaviors not captured in the current theory would change the formation mechanism of haze droplets, from the hygroscopic growth pathway to a nonclassical two-step nucleation pathway.

关键词： nanodroplet stability aerosol haze nucleation

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Experimental study on the space charge properties in haze events

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Journal of Environmental Sciences 2020年第1期32卷 361-376页

作者： Xiaobin Zhang Sen Yang Tianli Bo Key Laboratory of Mechanics on Western Disaster and Environment Lanzhou University

In recent years,haze has posed a serious threat to the global climate change,ecological balance and human *** this study,the laboratory experiments and field observations were performed and a possible charging mechanism was proposed to investigate the space charge properties in haze *** laboratory experiments showed that the charge polarity of primary aerosol is determined by species of combustion fuels while the magnitude is dependent on the combustion *** field observations revealed that the space charge of atmosphere aerosol in haze events differs from that of fair weather and is closely related to PM2.5 concentration when Relative Humidity(RH)haze events the space charge is governed by primary aerosol emitted by combustion of fossil fuel in a low relative humidity,whereas it is manipulated by the secondary chemical reaction of atmosphere aerosol in a high relative *** we can identify the main pollutants in haze events according to the polarity of atmosphere aerosol and quickly take measures when RHhaze of RHhaze when RHhaze when 60%≤RHhaze events and can provide a new perspective for the prevention and control of air pollution.

关键词： haze Atmosphere aerosol Space charge density(SCD) Equivalent charge-to-mass ratio(ECTM) Charging mechanisms

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Investigating the impact of Glyoxal retrieval from MAX-DOAS observations during haze and non-haze conditions in Beijing

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Journal of Environmental Sciences 2019年第6期31卷 296-305页

作者： Zeeshan Javed Cheng Liu Muhammad Fahim Khokhar Chengzhi Xing Wei Tan Muhammad Ahmed Subhani Abdul Rehman Aimon Tanvir School of Earth and Space Sciences University of Science and Technology of China Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Key Lab of Environmental Optics & Technology Anhui Institute of Optics and Fine Mechanics Chinese Academy of Sciences Anhui Province Key Laboratory of Polar Environment and Global Change USTC Institute of Environmental Sciences and Engineering National University of Sciences and Technology

This study presents the Multi Axis Differential Optical Absorption Spectroscopy(MAXDOAS) measurements for Glyoxal(CHOCHO) in Beijing, China(39.95°N, 116.32°E). CHOCHO is the smallest compound of di-carbonyl group. As a primary sink of CHOCHO, its photolysis with NOx(oxides of nitrogen) results in the production of tropospheric ozone. Therefore,the focus of CHOCHO DOAS measurements is increasing in trend. We did the measurements from 09 May 2017 to 09 September 2017. The study was conducted to compare different retrieval settings in order to reveal best DOAS fit settings for CHOCHO;furthermore, effect of haze and non-haze days on CHOCHO concentration was *** root mean square of residual and Differential Slant Column density(dSCD) error was reduced when measurements were done with lower wavelength limit around 432–438 nm and upper intervals around 455–460 nm. Thus, lower wavelength intervals around432–438 nm and upper intervals around 457–460 nm were best for the retrieval of dSCDs for CHOCHO. Meteorological conditions like haze or non-haze days did not have significant effect on DOAS fit parameters. The CHOCHO vertical column densities range from 1.33 E +14 to 9.77 E + 14 molecules/cm2 during the study period with average of 6.16 E +14 molecules/cm2. The results indicated that during haze days CHOCHO concentration was higher because of lower rate of photolysis and atmospheric oxidation potential. Our results did not show any significant weekend effect on CHOCHO atmospheric concentration.

关键词： Glyoxal DOAS Retrieval settings Photolysis haze days

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Observation of chemical components of PM2.5 and secondary inorganic aerosol formation during haze and sandy haze days in Zhengzhou, China

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Journal of Environmental Sciences 2020年第2期32卷 316-325页

作者： Zhangsen Dong Fangcheng Su Zhenya Zhang Shenbo Wang Graduate School of Life and Environmental Sciences University of TsukubaJapan Research Institute of Environmental Science College of Chemistry and Molecular EngineeringZhengzhou UniversityZhengzhou 450001China

Mineral dust particles play an important role in the formation of secondary inorganic aerosols, which largely contribute to haze pollution in *** this study, a haze episode(haze days) and a typical haze process mixed with sandstorm(sandy haze days)were observed in Zhengzhou with a series of high-time-resolution monitoring instruments from November 22 to December 8, *** of PM10 and crustal elements clearly increased in the sandy haze *** of gaseous pollutants, metallic elements emitted from anthropogenic sources, nitrate, and ammonium during sandy haze days were slightly lower than those during the haze days but still obviously higher than those during the non-haze *** sulfate concentrations, the sulfate fractions in PM2.5,and the sulfur oxidation ratios significantly increased in the sandy haze *** reactions dominated the conversion of SO2 during the haze and sandy haze *** SO2 conversion during the sandy haze days may be attributed to the high concentrations of transition metal ions from the sandstorm when the values of relative humidity(RH) were in 30%–70%, and high O3 at certain time ***-phase NO2 oxidation reactions were the main pathways for nitrate *** the sandy haze days,higher nitrogen oxidation ratio(NOR) at daytime may be associated with higher RH and lower temperature than those in the haze days, which facilitate the gas-to-particle partitioning of nitrate;higher NOR values at night may be attributed to the higher O3 concentrations, which promoted the formation of N2O5.

关键词： Sandstorm haze Sulfate Aqueous-phase reactions Transition metal ions

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Influence of rainfall-induced diabatic heating on southern rainfall-northern haze over eastern China in early February 2023

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Science China Earth Sciences 2023年第11期66卷 2579-2593页

作者： Xiadong AN Wen CHEN Chun LI Lifang SHENG Weihang ZHANG Shangfei HAI Peng HU Department of Marine Meteorology College of Oceanic and Atmospheric SciencesOcean University of ChinaQingdao 266100China Department of Atmospheric Sciences Yunnan UniversityKunming 650500China Yunnan Key Laboratory of Meteorological Disasters and Climate Resources in the Greater Mekong Subregion Yunnan UniversityKunming 650091China Center for Monsoon System Research Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100190China CMA Earth System Modeling and Prediction Center China Meteorological AdministrationBeijing 100081China

In early February 2023,there was severe haze on the North China Plain(NCP)that was contemporaneous with heavy rainfall over southern China,which was known as southern rainfall-northern haze(SR-NH).Based on observational and reanalysis data,the meteorological causes of this SR-NH event are investigated in this study using correlation analysis,dynamic diagnostics and numerical *** results show that the anticyclonic anomaly in the Pacific Northwest(also referred to as the northeast Asian anomalous anticyclone)is responsible for the *** the one hand,this anticyclonic anomaly leads to persistent rainfall over southern China by causing strong ascending motion in conjunction with an anomalous cyclone over the Chinese mainland and transporting large amounts of water vapor *** the other hand,it weakens the climatological northerly winds of the NCP through the southeasterly flow,worsening the horizontal diffusion conditions of ***,the atmospheric stability and relative humidity over the NCP are significantly increased by this anticyclonic *** conditions result in higher PM2.5concentrations over the *** results suggest that this anticyclonic anomaly is related to diabatic heating released by rainfall in southern China,which not only intensifies the rainfall process there(with a contribution of 11.5%)but also induces an anticyclonic anomaly in the upper troposphere of the Pacific Northwest(i.e.,200 hPa).The rainfall-related anticyclonic anomaly reinforces the anticyclonic anomaly in the Pacific Northwest caused by large-scale circulation(with a contribution of 27%)and thus affects haze over the *** study provides a new reference for understanding the contribution of rainfall in southern China to haze over the NCP.

关键词： Rainfall haze Diabatic heating Anticyclonic anomaly Eastern China

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Chemical compositions of PM_(2.5) aerosol during haze periods in the mountainous city of Yong'an, China

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Journal of Environmental Sciences 2012年第7期24卷 1225-1233页

作者： LiqianYin Zhenchuan Niu Xiaoqiu Chen Jinsheng Chen Lingling Xu Fuwang Zhang Key Laboratory of Urban Environment and Health Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Environmental Monitoring Center of Fujian Fuzhou 350003China Graduate School of Chinese Academy of Sciences Beijing 100049China

haze phenomena were found to have an increasing tendency in recent years in Yong＇an, a mountainous industrial city located in the center part of Fujian Province, China. Atmospheric fine particles （PM2.5） in the urban area during haze periods in three seasons （spring, autumn and winter） from 2007 to 2008 were collected, and the mass concentrations and chemical compositions （seventeen elements, water soluble inorganic ions （WSIIs） and carbonaceous species） of PM2.5 were determined. PM2.5 mass concentrations did not show a distinct difference among the three seasons. The carbonaceous species organic carbon （OC） and elemental carbon （EC） constituted up to 19.2%-30.4% of the PM2.5 mass during sampling periods, while WSIIs made up 25.3%-52.5% of the PM2.5 mass. The major ions in PM2.5 were SO42-, NO3- and NH4~, while the major elements were Si, K, Pb, Zn, Ca and A1. The experimental results （from data based on three haze periods with a 10-day sampling length for each period） showed that the crustal element species was the most abundant component of PM2.5 in spring, and the secondary ions species （SO42-, NO3-, NH4＋, etc.） was the most abundant component in PM2.5 in autumn and winter. This indicated that dust was the primary pollution source for PM2.5 in spring and combustion and traffic emissions could be the main pollution sources for PM2.5 in autumn and winter. Generally, coal combustion and traffic emissions were considered to be the most prominent pollution sources for this city on haze days.

关键词： PM2.5 haze metal elements water soluble inorganic ions carbonaceous species Yong'an City

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Review on formation mechanism analysis method and control strategy of urban haze in China

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Chinese Journal of Chemical Engineering 2019年第7期27卷 1572-1577页

作者： Weiqing Huang Lirong Cai Haifeng Dang Zhe Jiao Hongbo Fan Faliang Cheng School of Environment and Civil Engineering Guangdong Engineering and Technology Research Center for Advanced NanomaterialsDongguan University of TechnologyDongguan 523808China Guangdong Provincial Key Lab of Green Chemical Product Technology South China University of TechnologyGuangzhou 510640China

Due to the rapid urbanization and industrialization,and excessive consumption of fossil fuel,haze weather characterized by PM2.5 has become a severe pollution problem in major Chinese cities recently,which has harmful effect on the air quality,visibility,clime system and human *** indicate suitable directions for the prevention and control of haze pollution,the pollutant source apportionment and formation mechanism of urban haze should be figured out *** this work,we briefly review the frequently-used methods for PM2.5 source apportionment and formation mechanism analysis of urban haze based on normal perspective in recent ***,based on the new perspective of systematic methodology,the utilization of fault tree approach for the causation mechanism analysis of urban haze is significantly introduced and ***,the recent progress on controlling strategies of urban haze in China is also synoptically introduced and *** is expected that more effective tool/method can be found,developed and employed for the causation mechanism analysis and risk management of urban haze in China.

关键词： Urban haze Fossil fuel Formation Sustainability

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