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Journal of environmental Sciences 2024年第8期142卷 269-278页

作者： Ying Lu Se Wang Yifan Shen School of environmental Science and Engineering Collaborative Innovation Center of Atmospheric Environment and Equipment TechnologyJiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution ControlNanjing University of Information Science and TechnologyNanjing 210044China

The frequent detection of pharmaceutical compounds in the environment has led to a growing awareness,which may pose a major threat to the aquatic *** this study,photodegradation(direct and indirect photolysis)of two different dissociation states of fluoxetine(FLU)was investigated in water,mainly including the determination of photolytic transition states and products,and the mechanisms of indirect photodegradation with·OH,CO_(3)^(*-)and NO_(3)^(*).The main direct photolysis pathways are defluorination and C–C bond *** addition,the indirect photodegradation of FLU in water is mainly through the reactions with·OH and NO_(3)^(*),and the photodegradation reaction with CO_(3)^(*-)is relatively difficult to occur in the water *** results provide a theoretical basis for understanding the phototransformation process of FLU in the water environment and assessing its potential risk.

关键词： Fluoxetine Photochemical mechanism Direct photolysis Free radical reaction DFT

Development and evaluation of an online monitoring single-particle optical particle counter with polarization detection

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Journal of environmental Sciences 2024年第4期138卷 585-596页

作者： Weijie Yao Xiaole Pan Yu Tian Hang Liu Yuting Zhang Shandong Lei Junbo Zhang Yinzhou Zhang LinWu Yele Sun Zifa Wang State Key Laboratory of atmospheric Boundary Layer Physics and atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China center for Excellence in Regional atmospheric environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

We developed a single-particle optical particle counter with polarization detection(SOPC)for the real-time measurement of the optical size and depolarization ratio(defined as the ratio of the vertical component to the parallel component of backward scattering)of atmospheric particles,the polarization ratio(DR)value can reflect the irregularity of the *** SOPC can detect aerosol particles with size larger than 500 nm and the maximum particle count rate reaches~1.8×10^(5)particles per *** SOPC uses a modulated polarization laser to measure the optical size of particles according to forward scattering signal and the DR value of the particles by backward S and P signal *** sampling rate of the SOPC was 106#/(sec·channel),and all the raw data were processed *** calibration curve was obtained by polystyrene latex spheres with sizes of 0.5-10μm,and the average relative deviation of measurement was 3.96% for sub 3μm particles.T-matrix method calculations showed that the DR value of backscatter light at 120°could describe the variations in the aspect ratio of particles in the above size *** performed insitu observations for the evaluation of the SOPC,the mass concentration constructed by the SOPC showed good agreement with the PM_(2.5)measurements in a nearby state-controlled monitoring *** instrument could provide useful data for source appointment and regulations against air pollution.

关键词： Instrument development Single particle detection Measurement uncertainty Optical simulation Mass concentration

Development of an automatic measurement system using atmospheric pressure photoionization ultrahigh-resolution mass spectrometry and application for on-line analysis of particulate matter

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Journal of environmental Sciences 2024年第4期138卷 516-530页

作者： Yayuan Dong Ranran Liu Ling Xie Xiaole Pan Yele Sun Lin Wu ZifaWang State Key Laboratory of atmospheric Boundary Layer Physics and atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China center for Excellence in Regional atmospheric environment Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real *** we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS *** formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 *** a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the *** automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 *** detected organic compounds comprised mainly CHON and CHN compounds below 350 m/*** seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in *** result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in *** variation in signal intensity of each formula provides crucial information to reveal its source and formation *** summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).

关键词： PM_(2.5) Chemical composition On-line measurement technique High resolution mass spectrometry

The source of Double ITCZ induced by the SST bias over the tropical western Pacific as reflected in CAS-ESM2 Model

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Science China Earth Sciences 2024年第5期67卷 1604-1615页

作者： Jinning TONG Fei ZHENG Jiangbo JIN Ruowen YANG Jiang ZHU Qingcun ZENG Department of atmospheric Sciences Yunnan UniversityKunming 650091China International center for Climate and environment Science Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China

“Double ITCZ”is a common precipitation bias over the tropical Pacific in current climate models and Earth system models,but the reasons for its formation are still worth exploring and *** this study,we adopted the second version of Chinese Academy of Sciences Earth System Model(CAS-ESM2),by comparing a set of sea surface temperature(SST)bias correction experiments over the tropical Pacific,to explore the possible mechanism of SST bias on inducing the“Double ITCZ”from the perspective of the climatic annual mean bias in the coupled *** revealed that the simulated climatic annual mean SST bias over the tropical Pacific can affect the bias of latent heat flux through the saturation specific humidity,and the bias of latent heat flux can further affect that of vertical velocity of humid air by the condensation release mechanism,and finally modulate the simulated bias in ***,through the inter-comparison between different experiments,it is found that the source of Double ITCZ might mainly come from the annual mean SST bias over the tropical western Pacific through the proposed air-sea coupled process of“SST-saturated specific humidity-latent heat flux-vertical velocity-precipitation”,indicating a possible way on reducing the couple biases in models over the tropical Pacific to improve the accuracy of CAS-ESM2 for climate simulation.

关键词： SST bias Double ITCZ Nudging SST CAS-ESM2

Recent progress in carbene-catalyzed fluoroalkylation

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Science China Chemistry 2024年第8期67卷 2448-2460页

作者： Bei Zhang Xuan Zhang Jian Wang Jiangsu Key Laboratory of atmospheric environment Monitoring and Pollution Control Collaborative Innovation Center of Atmospheric Environment and Equipment TechnologySchool of Environmental Science and EngineeringNanjing University of Information Science and TechnologyNanjing 210044China School of Pharmaceutical Sciences Tsinghua UniversityBeijing 100084China

The fluoroalkyl fragment plays a vital role in various fields such as pharmaceuticals and materials science, and has a significant impact on human life not only on the present but also in the future. The insertion of fluoroalkyl groups into the chemical skeletons can cause considerable alternations in the chemical, physical and biological properties of molecules, which has attracted numerous scientists from different fields. This review focuses on N-heterocyclic carbene(NHC)-catalyzed fluoroalkylation reactions, providing a detailed analysis and summary of the achievements in the past two decades. Many successful examples clearly indicate that NHCs can catalyze the tranformation of fluoroalkylation reagents with various electronic characteristics, whether electrophilic, nucleophilic, or radical precursors. Herein, the fluoroalkylation reactions are classified based on different catalytic modes of NHCs: Lewis base catalysis, Umploung catalysis, radical catalysis and others. Meanwhile, by refining and systematically studying the contribution of NHC catalysis in fluoroalkylation reactions, this review is expected to provide valuable insights and enlightenment for related fields.

关键词： N-heterocyclic carbene fluoroalkylation radical catalysis

Excellent alkali resistance of Fe,Ce and sulfates co-modified V_(2)O_(5)-WO_(3)/TiO_(2) catalyst for selective catalytic reduction of NO_(x) with NH_(3)

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Journal of Rare Earths 2024年第9期42卷 1682-1692,I0002页

作者： Biyi Huang Xianfang Yi Jianyi Zhang Yuqiu Liu Yanting Chen Jinsheng Chen Jinxiu Wang center for Excellence in Regional atmospheric environment and Key Lab of Urban Environment and HealthInstitute of Urban EnvironmentChinese Academy of SciencesXiamen361021China College of Resources and environment Fujian Agriculture and Forestry UniversityFuzhou350002China Fujian Key Laboratory of atmospheric Ozone Pollution Prevention Institute of Urban EnvironmentChinese Academy of SciencesXiamen361021China University of Chinese Academy of Sciences Beijing100049China

Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a *** this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios *** NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of *** optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after *** interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox ***,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi ***,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on *** *** results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.

关键词： SCR CeO_(2) Fe_(2)O_(3) SO_(4)^(2-) K resistance K poisoning

Uncovering the dominant contribution of intermediate volatility compounds in secondary organic aerosol formation from biomass-burning emissions

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National Science Review 2024年第3期11卷 150-158页

作者： Kun Li Jun Zhang David M.Bell Tiantian Wang Houssni Lamkaddam Tianqu Cui Lu Qi Mihnea Surdu Dongyu Wang Lin Du Imad El Haddad Jay G.Slowik Andre S.H.Prevot environment Research Institute Shandong University Laboratory of atmospheric Chemistry Paul Scherrer Institute

Organic vapors from biomass burning are a major source of secondary organic aerosols(SOAs). Previous smog chamber studies found that the SOA contributors in biomass-burning emissions are mainly volatile organic compounds(VOCs). While intermediate volatility organic compounds(IVOCs) are efficient SOA precursors and contribute a considerable fraction of biomass-burning emissions, their contribution to SOA formation has not been directly observed. Here, by deploying a newly-developed oxidation flow reactor to study SOA formation from wood burning, we find that IVOCs can contribute ～70% of the formed SOA, i.e.>2 times more than VOCs. This previously missing SOA fraction is interpreted to be due to the high wall losses of semi-volatile oxidation products of IVOCs in smog chambers. The finding in this study reveals that SOA production from biomass burning is much higher than previously thought, and highlights the urgent need for more research on the IVOCs from biomass burning and potentially other emission sources.

关键词： atmospheric chemistry biomass burning secondary organic aerosol intermediate volatility organic compounds

Sources appointment and health risks of PM_(2.5)-bound trace elements in a coastal city of southeastern China

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Journal of environmental Sciences 2024年第4期138卷 561-571页

作者： Ziyi Lin Xiaolong Fan Gaojie Chen Youwei Hong Mengren Li Lingling Xu Baoye Hu Chen Yang Yanting Chen Zhiqian Shao Jinsheng Chen center for Excellence in Regional atmospheric environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Key Lab of Urban environment and Health Institute of Urban EnvironmentChinese Academy ofSciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China Minnan Normal University Zhangzhou 363000China

To gain a comprehensive understanding of sources and health risks of trace elements in an area of China with high population densities and low PM_(2.5)concentrations,15 trace elements(Al,K,Ca,Ti,V,Cr,Mn,Fe,Ni,Cu,Zn,As,Sn,Ba,Pb)in PM_(2.5)were monitored from December 2020 to November 2021 in a representative city,*** concentrations of trace elements in Xiamen displayed an obvious seasonal variation and were dominated by K,Fe,Al,Ca and *** on Positive Matrix Factorization analysis,source appointment revealed that the major sources of trace elements in Xiamen were traffic,dust,biomass and firework combustion,industrial manufacture and shipping *** to health risk assessment combined with the source appointment results,it indicated that the average noncarcinogenic risk was below the threshold and cancer risk of four hazardous metals(Cr,Ni,As,Pb)exceeded the threshold(10^(-6)).Traffic-related source had almost half amount of contribution to the health risk induced by PM_(2.5)-bound trace *** the dust transport period or Spring Festival period,the health risks exceeded an acceptable threshold even an order of magnitude higher,suggesting that the serious health risks still existed in low PM_(2.5)environment at certain *** risk assessment reminded that the health risk reduction in PM_(2.5)at southeastern China should prioritize traffic-related hazardous trace elements and highlighted the importance of controlling vehicles emissions in the future.

关键词： PM_(2.5)-bound trace elements Seasonal variations Source appointment Health risks Traffic-related source

Path signature-based XAI-enabled network time series classification

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Science China(Information Sciences) 2024年第7期67卷 91-106页

作者： Le SUN Yueyuan WANG Yongjun REN Feng XIA Department of Jiangsu Collaborative Innovation center of atmospheric environment and Equipment Technology(CICAEET) Nanjing University of Information Science and Technology School of Computing Technologies Royal Melbourne Institute of Technology

Classifying network time series(NTS) is crucial for automating network administration and ensuring cyberspace security. It enables the detection of anomalies, the identification of network attacks,and the monitoring of performance issues, thereby providing valuable support for network protection and optimization. However, modern communication networks pose challenges for NTS classification *** include handling large-scale and complex NTS data, extracting features from intricate datasets, and addressing explainability requirements. These challenges are particularly pronounced for complex 5G networks. Notably, explainability has become crucial for the widespread deployment of network automation for 5G networks and beyond. To tackle these challenges, we propose a path-signature-based NTS classification model called recurrent signature(Recur Sig). This innovative model is designed to overcome the time-consuming feature selection problem by utilizing deep-learning(DL) techniques. Additionally, it provides a solution for addressing the black-box issue associated with DL models in network automation systems(NAS) by incorporating an explainable classification approach. Extensive experimentation on various public datasets demonstrates that Recur Sig outperforms existing models in accuracy and explainability. The results indicate its potential for application in cyberspace security and automated network management, offering an explainable solution for network protection and optimization.

关键词： network time series classification explainable artificial intelligence path signature automated network management recurrent neural network

Climatic drivers of the Canadian wildfire episode in 2023

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atmospheric and Oceanic Science Letters 2024年第4期17卷 23-28页

作者： Yihan Hu Xu Yue Chenguang Tian Jiangsu Key Laboratory of atmospheric environment Monitoring and Pollution Control Collaborative Innovation Center of Atmospheric Environment and Equipment TechnologySchool of Environmental Science and EngineeringNanjing University of Information Science&Technology(NUIST)NanjingChina

2023年5月加拿大发生极端野火事件并持续4个月时间.野火污染物排放对当地和下风向的空气质量造成了严重影响.本文对驱动此次野火事件的气象因子和相关大尺度环流进行了探究.研究表明,此次极端野火排放的二氧化碳相较往年同期增长了0.37G... 详细信息

2023年5月加拿大发生极端野火事件并持续4个月时间.野火污染物排放对当地和下风向的空气质量造成了严重影响.本文对驱动此次野火事件的气象因子和相关大尺度环流进行了探究.研究表明,此次极端野火排放的二氧化碳相较往年同期增长了0.37Gt (527.1%).受罗斯贝波频散影响,同期加拿大中西部区域出现持续的位势高度正异常,促进气流下沉并引发局地高温,中西部区域5-6月最高温平均上升8.11℃,部分区域甚至超过10℃,导致野火排放的显著增长.受有利地形和泛北极地区快速增暖的影响,预期未来加拿大中西部发生极端野火的概率可能会显著上升.

关键词：野火气候变化遥相关极端天气碳排放