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Organic peroxyl radicals from biacetyl accelerated the visible-light degradation of steroid estrogens in aqueous solution

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Chemosphere 2024年 351卷 141195页

作者： Jia, Yulu Zhang, Chengyang Zheng, Hongcen Zhang, Guoyang Zhang, Shujuan State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China

Indirect photodegradation is an important pathway for the reduction of steroid estrogens in sunlit surface waters. Nevertheless, the kinetics and mechanisms governing the interaction between coexisting carbonyl compounds and estrogens under visible light (Vis) remain unexplored. This study systematically investigates the Vis-induced photodegradation of 17β-estradiol (E2) in the presence of five specific carbonyl compounds—biacetyl (BD), acetone, glyoxal, pyruvic acid, and benzoquinone. The results demonstrate that, among these compounds, only BD significantly enhanced the photodegradation of E2 under Vis irradiation (λ > 400 nm). The pseudo-first order photodegradation rate constants (k1) of E2 in the Vis/BD system were 0.025 min−1 and 0.076 min−1 in ultrapure water and river water, respectively. The enhancing effect of BD was found to be pH-dependent, increasing the pH from 3.0 to 11.0 resulted in a 76% reduction in the k1 value of E2 in the Vis/BD system. Furthermore, the presence of humic acid, NO3−, or HCO3− led to an increase of more than 35% in the k1 value of E2, while NO2− exerted a pronounced inhibitory effect, resulting in a 92% decrease. Peroxyacetyl and peroxymethyl radicals, derived from BD in a yield ratio of 9, played a crucial role in the degradation of E2. These peroxyl radicals primarily targeted electron-rich hydroxyl sites of E2, initiating hydroxylation and ring-opening reactions that culminated in the formation of acidic byproducts. Notably, toxicity evaluation indicates that these hydroxylated and acidic products exhibited lower toxicity than the parent compound E2. This study highlights the important role of peroxyl radicals in estrogen degradation within aquatic environment, and also helps to design efficient visible light-responsive photo-activators for the treatment of estrogen-contaminated waters. © 2024 Elsevier Ltd

关键词： Photolysis

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Improved atmospheric mercury simulation using updated gas-particle partition and organic aerosol concentrations

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Journal of Environmental Sciences 2022年第9期34卷 106-118页

作者： Kaiyun Liu Qingru Wu Shuxiao Wang Xing Chang Yi Tang Long Wang Tonghao Liu Lei Zhang Yu Zhao Qin’geng Wang Jinsheng Chen State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084China Institute of Atmospheric Environment Guangdong provincial academy of environmental scienceGuangzhou 510045China China National Environmental Monitoring Centre Beijing 100012China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing210023China Center for Excellence in Regional Atmos.Environ. Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

The gaseous or particulate forms of divalent mercury(HgⅡ) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux(FLX). In the new nested-grid GEOS-Chem model, we try to modify the HgⅡ gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg(GOM), particulate-bound Hg(PBM), and PM 2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature( T) and organic aerosol(OA) concentrations under different relative humidity(RH). Results showed that with increasing RH, the dominant process of HgⅡ gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgⅡ gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds(I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases(NMBs) of monthly gaseous element mercury(GEM), GOM, PBM, WFLX were reduced from-33%–29%, 95%–300%, 64%–261%, 117%–122% to-13%–0%,-20%–80%,-31%–50%,-17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.

关键词： Nested GEOS-Chem model HgⅡgas-particle partitioning Organic aerosol Atmospheric mercury Mercury deposition flux

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A study on singlet oxygen generation for tetracycline degradation via modulating the size ofα-Fe_(2)O_(3)nanoparticle anchored on g-C_(3)N_(4) nanotube photocatalyst

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Nano Research 2023年第2期16卷 2236-2244页

作者： Hongjie Zhu Minghui Li Luning Zou Youyou Hu Hongguo Hao Jianmin Dou Junjie Mao Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252059China Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Gaotang liguo chemical plant Liaocheng 252059China

Photocatalysis is considered as an effective technique for mitigating ecological risks posed by residual tetracycline(TC).To improve the efficiency of this technique,it is necessary to enable photocatalysts to produce highly reactive species,such as singlet oxygen(1O2).However,due to the high activation energy of 1O2,photocatalysts can hardly produce 1O2 without assistance from external ***,we find that the size-reducedα-Fe_(2)O_(3)nanoparticles(~4 nm)that anchored on g-C_(3)N_(4)nanotube(α-Fe_(2)O_(3)@CNNT)can spontaneously generate ^(1)O_(2) for degradation of *** comparison,only hydroxyl radical(·OH)can be produced by g-C_(3)N_(4)nanotube loaded with~14 nmα-Fe_(2)O_(3)nanoparticles(α-Fe_(2)O_(3)/CNNT).Owing to the high reactivity of the ^(1)O_(2) species,the photocatalytic degradation rate(Kapp)of TC withα-Fe_(2)O_(3)@CNNT(0.056 min^(−1))was 1.8 times higher than that ofα-Fe_(2)O_(3)/*** experimental results and theoretical calculations suggested that reducing the size ofα-Fe_(2)O_(3)nanoparticles anchored on g-C_(3)N_(4)nanotube decreased the surface electron density ofα-Fe_(2)O_(3),which induces the generation of high-valent Fe(IV)active sites overα-Fe_(2)O_(3)@CNNT and turns the degradation pathway into a unique ^(1)O_(2) dominated *** study provides a new insight on the generation of ^(1)O_(2) for effective degradation of environmental pollutant.

关键词： singlet oxygen degradation pathway high-valent Fe(IV) tetracycline degradation

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Evidence on the causes of the rising levels of COD_(Mn) along the middle route of the South-to-North Diversion Project in China:The role of algal dissolved organic matter

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Journal of Environmental Sciences 2022年第3期34卷 281-290页

作者： Chao Wang Hong Zhang Pei Lei Xiaokang Xin Aijing Zhang Wei Yin Changjiang Water Resources Protection Institute Wuhan 430051China State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China State Key Laboratory of Pollution Control and Resources Reuse School of the EnvironmentNanjing UniversityNanjing 210046China Construction and Administration Bureau of South-to-North Water Diversion Middle Route Project Beijing 100038China Key Laboratory cf Ecological Regulation ofNon-point Source Pollution in Lake and Reservoir Water Sources Wuhan 430051China

As the biggest inter-basin water transfer scheme in the world,the South-to-North Water Diversion Project(SNWD) was designed to alleviate the water crisis in North *** main channel of the middle route of the SNWD is of great concern in terms of the drinking water *** this study,we tested the hypothesis that the dissolved organic matter(DOM) derived from the planktonic algae causes the rising levels of COD_(Mn) along the middle route by monitoring data on water quality(2015-2019,monthly resolution).The results showed that algal density in the main channel increased along the channel and was significantly correlated with COD_(Mn)(p <0.01).Five fluorescent components of DOM,including tyrosine-like(14.85%),tryptophan-like(22.48%),microbial byproduct-like(26.34%),fulvic acid-like(11.41%),and humic acid-like(24.92%) components,were *** level of tyrosine-like components increased along the channel and was significantly correlated with algal density(p<0.01),indicating that algae significantly changed the level of DOM in the *** decomposition and metabolism were found to be the main mechanisms that drive the changes in COD_(Mn).Therefore,controlling algal density would be an important measure to prevent further increase in CODMn and for the guarantee of excellent water quality.

关键词： Dissolved organic matter(DOM)Algae COD_(Mn) South-to-North Diversion Project Danjiangkou reservoir Three-dimensional fluorescence excitation emission matrix spectroscopy(3D-EEMs)

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A MISR-Based Method for the Estimation of Particle Size Distribution:Comparison with AERONET over China

Journal of Remote Sensing

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Journal of Remote Sensing 2023年第1期3卷 97-109页

作者： Yanchuan Shao Riyang Liu Weihan Li Jun Bi Zongwei Ma State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjingJiangsuChina Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology(CICAEET) Nanjing University of Information Science&TechnologyNanjingJiangsuChina

Aerosol particle size has a crucial impact on the environment and public *** satellite-based regression models focus on the total amount of particles and are limited by surface *** study proposes an algorithm to derive the long-term normalized volume size distribution(VSD)of aerosol particles,which is independent of ground *** size distribution and aerosol optical depth of Multi-angle Imaging SpectroRadiometer(MISR)components are *** find the estimated MISR VSD is consistent with Aerosol Robotic Network(AERONET)observations,with R=0.56,0.54,0.59,and 0.68 for daily,monthly,seasonal,and annual *** stratified validations of radius,stations,and years further confirm the stable performance of derived VSD(R=0.28 to 0.73).The application of the random forest model demonstrates the potential improvements of predicted VSD by 10-fold cross-validation R=0.86 at the monthly *** apply MISR VSD to quantify the normalized volume of fractional aerosol particles at a resolution of 0.2°×0.2°during 2004 to 2016 in *** also calculate the proportion of small and medium particles to indicate the contribution of anthropogenic *** highest ratios are concentrated in the northeastern regions especially during winter while relatively lower in the Taklamakan Desert of western *** case study demonstrates that the application of MISR data can yield valuable and resolved size distributions of aerosol particles.

关键词： AERONET aerosol MISR

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Research progress of nitrate removal technologies based on photoelectrochemical reduction

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Zhongguo Huanjing Kexue/China Environmental Science 2025年第4期45卷 1878-1888页

作者： Huang, Tian-Rong Wang, Kai-Chong Li, Zi-Bin Li, Dan-Ping Wang, Han Wang, Ya-Yi School of Environmental Science and Engineering Tongji University Shanghai200092 China State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai200092 China

As a common pollutant in water, nitrate has nonnegligible harmful effects on human health and the ecological environment. Faced with an increasingly severe energy crisis, the development of green, clean and sustainable nitrate removal technologies to replace the conventional resource-intensive denitrification process is urgently needed. Photoelectrochemical nitrate reduction powered by sunlight has become a research hotspot at home and abroad. Based on the way photogenerated electrons being transferred from semiconductor to nitrate, this technology can be categorized into photocatalytic reduction, photoelectrocatalytic reduction, and microbial photoelectrotrophic reduction. In this review, the mechanisms of three photoelectrochemical nitrate reduction technologies were discussed. With a focus on improving system performance, the selection and design strategies of photocatalysts, photoelectrodes and microbial photosensitizers were also summarized. Moreover, the technical difficulties of photoelectrochemical nitrate reduction are clarified and the future directions of research are proposed, such as regulating the pathway of microbial absorption and utilization of photogenerated electrons through genetic engineering and other methods. The insights provided will serve as a reference for the development of new nitrate removal and reutilization technologies. © 2025 Chinese Society for Environmental Sciences. All rights reserved.

关键词： Sustainable development

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Coastal mudflats as reservoirs of extracellular antibiotic resistance genes: Studies in Eastern China

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Journal of Environmental Sciences 2023年第7期129卷 58-68页

作者： Qingbin Yuan Xiaolin Wang Hui Fang Yuan Cheng Ruonan Sun Yi Luo College of Environmental Science and Engineering Nanjing Tech UniversityNanjing 211816China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China School of Medicine Nankai UniversityTianjin 300071China Department of Civil and Environmental Engineering Rice UniversityHouston 77005USA

Despite coastal mudflats serving as essential ecological zones interconnecting terrestrial/freshwater and marine systems,little is known about the profiles of antibiotic resistance genes(ARGs)in this *** this study,characteristics of typical ARGs,involving both intracellular(iARGs)and extracellular ARGs(eARGs)at different physical states,were explored in over 1000 km of coastal mudflats in Eastern *** indicated the presence of iARGs and eARGs at states of both freely present or attached by *** abundance of eARGs was significantly higher than that of iARGs(87.3%vs 12.7%),and their dominance was more significant than those in other habitats(52.7%-76.3%).ARG abundance,especially for eARGs,showed an increasing trend(p<0.05)from southern(Nantong)to northern(Lianyungang)*** salinity facilitated the transformation from iARGs to eARGs,and smaller soil particle size was conducive to the persistence of eARGs in northern coastal *** study addresses the neglected function of coastal mudflats as eARGs reservoirs.

关键词： Antibiotic resistance genes(ARGs) Extracellular antibiotic resistance genes(eARGs) Coastal mudflats Amplicon sequencing Geochemical variable Mobile genetic elements

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Effect of nitrite on hydrolysis-acidification, biogas production and microbial community in semi-continuous two-phase anaerobic digestion of sewage sludge

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Journal of Environmental Sciences 2023年第4期126卷 434-444页

作者： Qian Sheng Yiqing Lu Shijie Yuan Xiaowei Li Xiaohu Dai Yali Guo Bin Dong State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China School of Environmental and Chemical Engineering Organic Compound Pollution Control EngineeringMinistry of EducationShanghai UniversityShanghai 200444China Shanghai Investigation Design&Research Institute Co.Ltd. Shanghai 200335China YANGTZE Eco-Environment Engineering Research Center China Three Gorges CorporationBeijing 100038China

Previous study found that the pre-treatment of sewage sludge with nitrite improves the biogas production during the mono/two-phase anaerobic digestion (AD) using batch biochemical methane potential *** this study,the effects of nitrite on hydrolysisacidification,biogas production,volatile solids destruction and microbial composition in semi-continuous two-phase AD of sewage sludge were *** addition of nitrite promotes sludge organic matter solubilization (+484%) and VFAs production (+98.9%),and causes an increase in the VS degradation rate during the AD process (+8.7%).The comparison of biogas production from the acidogenic and methanogenic reactors with or without the addition of nitrite implies that the nitrite has no significant effect on the overall biogas production of two-phase sludge AD ***-throughput sequencing analysis shows that the microbial communities of bacteria and archaea in two-phase AD reactors significantly changes after the addition of *** (bacteria) and Candidatus Methanofastidiosum (archaea) become the dominant genera in the acidogenic and methanogenic reactors with the nitrite *** findings provide new insights about using nitrite to promote the organic matter degradation of sewage sludge in a semicontinuous two-phase AD system.

关键词： Sewage sludge Bioenergy Methane production Nitrite Semi-continuous two-phase anaerobic digestion

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Microplastics in landfill leachate:sources,detection,occurrence,and removal

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Environmental Science and Ecotechnology 2023年第4期16卷 26-37页

作者： Mosarrat Samiha Kabir Hong Wang Stephanie Luster-Teasley Lifeng Zhang Renzun Zhao Department of Nanoengineering North Carolina Agricultural and Technical State UniversityGreensboroNC27411USA State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China Civil Architectural and Environmental Engineering DepartmentNorth Carolina Agricultural and Technical State UniversityGreensboroNC27411USA

Due to the accumulation of an enormous amount of plastic waste from municipal and industrial sources in landfills,landfill leachate is becoming a significant reservoir of *** release of microplastics from landfill leachate into the environment can have undesirable effects on humans and *** study provides the state of the science regarding the source,detection,occurrence,and remediation of microplastics in landfill leachate based on a comprehensive review of the scientific literature,mostly in the recent *** waste and wastewater treatment residue are the primary sources of microplastics in landfill *** concentration in raw and treated landfill leachate varied between 0-382 and 0-2.7 items L^(−1).Microplastics in raw landfill leachate are largely attributable to local plastic waste production and solid waste management ***,polystyrene,and polypropylene are the most prevalent microplastic polymers in landfill *** though the colors of microplastics are primarily determined by their parent plastic waste,the predominance of light-colored microplastics in landfill leachate indicates long-term *** identified morphologies of microplastics in leachate from all published sources contain fiber and fragments the *** on the treatment method,leachate treatment processes can achieve microplastic removal rates between 3%and 100%.The review also provides unique perspectives on microplastics in landfill leachate in terms of remediation,final disposal,fate and transport among engineering systems,and source reduction,*** landfill-wastewater treatment plant loop and bioreactor landfills present unique difficulties and opportunities for managing microplastics induced by landfill leachate.

关键词： Landfill leachate Microplastics source Detection Occurrence Treatment

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Hydrogeochemical characteristics and potential risks within a headwater catchment， Taihu Lake Basin， China

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Journal of Earth Science 2024年

作者： Lin Liu Hai Yang Xun Zhou Yuehua Jiang Naizheng Xu Jiangshi Gong Zi Chen Liang Li Jinsong Lv Yang Jin Chinese Academy of Geological Sciences Nanjing Center China Geological Survey Key Laboratory of Watershed Eco-Geological Processes， Ministry of Natural Resources State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution， China University of Geosciences(Wuhan)

The Yuying River catchment is a hilly watershed that serves as a high-quality water source for Taihu Lake. Its hydrochemical characteristics is crucial to the safety of water supplies around Taihu Lake. In order to evaluate the potantial risk to Taihu Lake， samples of rainwater， surface water， and groundwater from the Yuying River catchment were gathered to conduct a comprehensive hydrochemical analysis， the isotope analysis of δ2H， δ18O， and3H. The results showed that the hydrochemical types of the groundwater were mainly HCO3·SO4-Na·Ca and HCO3-Na·Ca. The renewal rate of groundwater in the Yuying River catchment is slightly greater （+10% to +20%） than 34% a-1. The formation process of hydrochemical characteristics was controlled by the process of cation exchange and leaching （mainly based on silicate dissolution）. Combined with historical data， the concentration of NO3-in groundwater of the Yuying River catchment was increased from 2000（4.7 mg/L） to 2019（15.8 mg/L）. Both the constructed land area （increase 377.31%） and NO3-concentration in groundwater （increase 336.17%） elevated about 3 times compared with thoses in 2000. Combined with PCA statistical analysis of nitrate in groundwater of different land use， it was found that the discharge of domestic sewage was the main reason of the abnormal increase of NO3-in the study area. It suggested that the enhanced of human activities （unscientific domestic sewage disposal） has exceeded the self-purification ability of the Yuying river catchment water environment. It is urgent to adopt scientific and effective domestic sewage treatment methods to ensure the water environment and water ecological security of the Yuying river catchment and the downstream Taihu Lake.

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