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Chinese Journal of Chemical Engineering 2024年第4期68卷 27-34页

作者： Xi Quan Jun Zhang Linlin Yin Wei Zuo Yu Tian state key laboratory of urban water Resource and environment(skluwre) School of EnvironmentHarbin Institute of TechnologyHarbin 150090China

In this work,a novel composite material based on β-cyclodextrin-immobilized sodium alginate aerogel(β-CD/NaAlg) was developed utilizing cross-linker of epichlorohydrin and applied as an adsorbent to remove tetracycline antibiotics from reclaimed wastewater.A series of characterizations were utilized to confirm the successful synthesis of the adsorbent and this β-CD/NaAlg presented a three-dimensional network at the nanoscale or microscale.Under optimal conditions(pH=4,t=8 h,β-CD:NaAlg=9,adsorbent dosage = 1.5 g·L-1),the maximum removal rate of β-CD/NaAlg to tetracycline was 70%.The adsorption behavior of tetracycline on β-CD/NaAlg conformed to the Freundlich isotherm model(R2=0.9977) and the pseudo-second-order kinetic model(R^(2)=0.9993).Moreover,the adsorbent still removed 55.3% of tetracycline after five cycles.Specially,the adsorbent was integrated with ultrafiltration to adsorb tetracycline antibiotics from simulated reclaimed wastewater,and the removal rate of tetracycline reached 78.9% within 2 h.The existence of Cr(Ⅵ) had a negligible impact on tetracycline removal,while the presence of humic acid exhibited a promoting effect.The possible adsorption mechanisms were also elucidated through X-ray photoelectron spectroscopy and density functional theory analysis.In summary,β-CD/NaAlg represents an environmentally friendly,efficient,and sustainable adsorbent for removing tetracycline antibiotics from reclaimed water.

关键词： b-CD/NaAlg aerogel Covalent grafting Tetracycline antibiotics Ultrafiltration Selective adsorption Reclaimed water

Mechanistic insight into Cr(Ⅵ)retention by Si-containing ferrihydrite

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Journal of environmental Sciences 2024年第5期139卷 217-225页

作者： Ying Hu Qiang Xue Honghan Chen Huaming Guo Kenneth C.Carroll Song Wang MOE key laboratory of Groundwater Circulation and environmental Evolution School of Water Resources and EnvironmentChina University of Geosciences(Beijing)Beijing 100083China Beijing key laboratory of water resources and environmental Engineering School of Water Resources and EnvironmentChina University of GeosciencesBeijing 100083China state key laboratory of Biogeology and environmental Geology China University of GeosciencesBeijing 100083China Plant&environmental Science New Mexico State UniversityNM 88003USA Institute of Theoretical Chemistry College of ChemistryJilin UniversityChangchun 130023China

Hexavalent chromium[Cr(Ⅵ)]causes serious harm to the environment due to its high toxicity,solubility,and mobility.Ferrihydrites(Fh)are the main adsorbent and trapping agent of Cr(Ⅵ)in soils and aquifers,and they usually coexist with silicate(Si),forming Si-containing ferrihydrite(Si-Fh)mixtures.However,the mechanism of Cr(Ⅵ)retention by Si-Fh mixtures is poorly understood.In this study,the behaviors and mechanisms of Cr(Ⅵ)adsorption onto Si-Fh with different Si/Fe molar ratios was investigated.Transmission electron microscope,Fourier transform infrared spectroscopy,X-ray diffraction,X-ray photoelectron spectroscopy,and other techniques were used to characterize Si-Fh and Cr(Ⅵ)-loading of Si-Fh.The results show that specific surface area of Si-Fh increases gradually with increasing Si/Fe ratios,but Cr(Ⅵ)adsorption on Si-Fh decreases with increasing Si/Fe ratios.This is because with an increase in Si/Fe molar ratio,the point of zero charge of Si-Fh gradually decreases and electrostatic repulsion between Si-Fh and Cr(Ⅵ)increases.However,the complexation of Cr(Ⅵ)is enhanced due to the increase in adsorbed hydroxyl(A-OH-)on Si-Fh with increasing Si/Fe molar ratio,which partly counteracts the effect of the electrostatic repulsion.Overall,the increase in the electrostatic repulsion has a greater impact on adsorption than the additional complexation with Si-Fh.Density functional theory calculation further supports this observation,showing the increases in electron variation of bonding atoms and reaction energies of inner spherical complexes with the increase in Si/Fe ratio.

关键词： Hexavalent chromium Ferrihydrite Si/Fe ratio Cr(Ⅵ)Adsorption

Influence of meteorological factors on open biomass burning at a background site in Northeast China

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Journal of environmental Sciences 2024年第4期138卷 1-9页

作者： Yulong Wang Linlin Liang Wanyun Xu Chang Liu Hongbing Cheng Yusi Liu Gen Zhang Xiaobin Xu Dajiang Yu Peng Wang Qingli Song Jiumeng Liu Yuan Cheng state key laboratory of urban water Resource and environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China state key laboratory of Severe Weather&key laboratory for Atmospheric Chemistry Chinese Academy of Meteorological SciencesBeijing 100081China Longfengshan Regional Background Station China Meteorological AdministrationHeilongjiang 150200China Heilongjiang Climate Center Heilongjiang 150030China

Biomass burning(BB)is a very important emission source that significantly adversely impacts regional air quality.BB produces a large number of primary organic aerosol(POA)and black carbon(BC).Besides,BB also provides many precursors for secondary organic aerosol(SOA)generation.In this work,the ratio of levoglucosan(LG)to organic carbon(OC)and the fire hotspots map was used to identify the open biomass burning(OBB)events,which occurred in two representative episodes,October 13 to November 30,2020,and April1 to April 30,2021.The ratio of organic aerosol(OA)to reconstructed PM_(2.5)concentration(PM_(2.5)^(*))increased with the increase of LG/OC.When LG/OC ratio is higher than 0.03,the highest OA/PM_(2.5)^(*)ratio can reach 80%,which means the contribution of OBB to OA is crucial.According to the ratio of LG to K^(+),LG to mannosan(MN)and the regional characteristics of Longfengshan,it can be determined that the crop residuals are the main fuel.The occurrence of OBB coincides with farmers’preferred choices,i.e.,burning biomass in“bright weather”.The“bright weather”refers to the meteorological conditions with high temperature,low humidity,and without rain.Meteorological factors indirectly affect regional biomass combustion pollution by influencing farmers’active choices.

关键词： Air pollution Biomass burning Meteorological factors Organic trace Agricultural fires

urban water system theory and its model development and application

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Science China Earth Sciences 2024年第3期67卷 704-724页

作者： Jun XIA Yongyong ZHANG Dunxian SHE Shiyan ZHANG Jun YANG Mingquan LV Xiang ZHANG Anqi LUO Shengjun WU Yang LIU key laboratory of water Cycle and Related Land Surface Processes Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of SciencesBeijing 100101China state key laboratory of water resources&Hydropower Engineering Sciences Wuhan UniversityWuhan 430072China Aquatic Eco Health Group Key Laboratory of Urban Environment and HealthInstitute of Urban EnvironmentFujian Key Laboratory of Watershed EcologyChinese Academy of SciencesXiamen 361021China Chongqing Institute of Green and Intelligent Technology Chinese Academy of SciencesChongqing 400714China

The urban water system theory is an extension of the basin water system science on an urban scale, providing a new systematic solution for the unbalanced human-water relationship and severe water challenges, such as waterlogging, black and odorous water, and ecological degradation caused by urbanization. Most existing studies on urban water systems have focused on individual water cycle processes linked with water supply and sewage treatment plants, but mutual feedback between the water cycle and its associated material circulation and water ecology, as well as human processes, still needs further exploration. In this paper, the concept, theory, and technical methodology of the urban water system were developed based on the water cycle and basin water system science. The urban water System 5.0(UWS 5.0) model was developed by integrating the Time Variant Gain rainfall-runoff Model with urban water system(TVGM_urban) in different underlying surface conditions for analyzing the natural-social water cycle processes and their associated water environmental and ecological processes and the influence of multiscale sponge measures. Herein, five major simulation functions were realized: rainfall-runoff-nonpoint source pollutant load,water and pollutant transportations through the drainage network system, terminal regulation and purification, socioeconomic water cycle, and water system assessment and regulation. The location for the case study used in this paper was Wuhan City. The findings showed that the entire urban water system should consider the built-up area and its associated rivers and lakes as the research object and explore the integrations among the urban natural-social water cycle and river regulations inside and outside of the city as well as the effects of socioeconomic development and sponge measures on the water quantity-quality-ecology processes. The UWS 5.0 model efficiently simulated the urban rainfall-runoff process, total nitrogen(TN) and total phosphorus(TP) concentrations in water bodies, and charac

关键词： urban water system Human-water relationship water issue Green development Theoretical basis Mathematical model

Spatial heterogeneity and compositional profiles of dissolved organic matter in farmland soils across China' Mainland

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Journal of environmental Sciences 2024年第3期137卷 593-603页

作者： Bingjun Han Liyuan Chen Kang Xiao Yang Liu Dong Cao Lu Yu Yujun Li Shu Tao Wenxin Liu key laboratory for Earth Surface Processes College of Urban and Environmental SciencesPeking UniversityBeijing 100871China Beijing Yanshan Earth Critical Zone National Research Station College of Resources and EnvironmentUniversity of Chinese Academy of SciencesBeijing 101408China Center for water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China state key laboratory of environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental ScienceChinese Academy of SciencesBeijing 100085China

Dissolved organic matter(DOM) plays an essential role in many geochemical processes,however its complexity, chemical diversity, and molecular composition are poorly understood. Soil samples were collected from 500 vegetable fields in administrative regions of China' Mainland, of which 122 were selected for further investigation. DOM properties were characterized by three-dimensional excitation-emission matrix(3D-EEM) fuorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry(FTICRMS)(field intensity is 15 Tesla). Our results indicated that the main constituents were UVA humic-like substances, humic-like substances, fulvic acid-like substances, and tyrosine-like substances. A total of 10,989 molecular formulae with a mass range of 100.04 to 799.59 Da were detected, covering the mass spectrometric information of the soil samples from 27 different regions. CHO and CHON molecules were dominant in DOM, whereas lignin, tannins,and aromatic substances served as the main components. The results of cluster analysis revealed that the soil properties in Jiangxi Province were considerably different from those in other regions. The key backgrounds of the DOM molecular characteristics in the vegetablefield soil samples across China' Mainland were provided at the molecular level, with large abundance and great variability.

关键词： Dissolved organic matter(DOM) Fourier transform ion cyclotron resonance mass(FTICR-MS) Excitation-emission matrix(EEM) Vegetable-field soils China' Mainland

Iron–doped bismuth oxybromides as visible-light-responsive Fenton catalysts for the degradation of atrazine in aqueous phases

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Journal of environmental Sciences 2024年第3期137卷 321-332页

作者： Yong-Li Cai Yu-Hang Xu Ji-Zun Xiang Zhi-Qiang Zhang Qiu-Xiang He Ya-Feng Li Jian Lü Fujian Provincial key laboratory of Soil environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China state key laboratory of Photocatalysis on Energy and environment Fuzhou UniversityFuzhou 350116China

Pesticides and its degradation products,being well–known residues in soil,have recently been detected in many water bodies as pollutants of emerging concerns,and thus there is a contemporary demand to develop viable and cost–effective techniques for the removal of related organic pollutants in aqueous phases.Herein,a visible-light-responsive Fenton system was constructed with iron–doped bismuth oxybromides(Fe–BiOBr)as the catalysts.Taking the advantage of sustainable Fe(Ⅲ)/Fe(Ⅱ)conversion and optimized H_(2)O_(2)utilization,the optimal Fe–BiOBr–2 catalyst showed an excellent atrazine removal efficiency of 97.61%in 120 min,which is superior than the traditional homogeneous Fenton and the majority of heterogeneous processes documented in the literature.In this photo–Fenton system,hydroxyl(·OH)and superoxide(·O_(2)^(-))radicals were dominant active species contributed to the oxidative degradation of atrazine.Due to the production of various active radicals,five degradation pathways were proposed based on the identification of intermediates and degradation products.Overall,this work not only demonstrates a fundamental insight into creating highly efficient and atom economic photo-Fenton systems,but also provides a complementary strategy for the treatment of organic pollutants in water.

关键词： Bismuth oxybromide Photo–Fenton Atrazine Catalytic degradation

Nitrogen-doped titanium dioxide/schwertmannite nanocomposites as heterogeneous photo-Fenton catalysts with enhanced efficiency for the degradation of bisphenol A

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Journal of environmental Sciences 2024年第9期143卷 1-11页

作者： Xing-Xing Qiao Yu-Hang Xu Xiang-Ji Liu Sai-Le Chen Zhou Zhong Ya-Feng Li Jian Lü Fujian Provincial key laboratory of Soil environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China state key laboratory of Photocatalysis on Energy and environment Fuzhou UniversityFuzhou 350116China

Potential health risks related to environmental endocrine disruptors(EEDs)have aroused research hotspots at the forefront of water treatment technologies.Herein,nitrogen-doped titanium dioxide/schwertmannite nanocomposites(N-TiO_(2)/SCH)have been successfully developed as heterogeneous catalysts for the degradation of typical EEDs via photo-Fenton processes.Due to the sustainable Fe(Ⅲ)/Fe(Ⅱ)conversion induced by photoelectrons,as-prepared N-TiO_(2)/SCH nanocomposites exhibit much enhanced efficiency for the degradation of bisphenol A(BPA;ca.100% within 60 min under visible irradiation)in a wide pH range of 3.0-7.8,which is significantly higher than that of the pristine schwertmannite(ca.74.5%)or N-TiO_(2)(ca.10.8%).In this photo-Fenton system,the efficient degradation of BPA is mainly attributed to the oxidation by hydroxyl radical(·OH)and singlet oxygen(^(1)O_(2)).Moreover,the possible catalytic mechanisms and reaction pathway of BPA degradation are systematically investigated based on analytical and photoelectrochemical analyses.This work not only provides a feasible means for the development of novel heterogeneous photo-Fenton catalysts,but also lays a theoretical foundation for the potential application of mineral-based materials in wastewater treatment.

关键词： Titanium dioxide Schwertmannite Fenton reaction environmental endocrine disruptors Photocatalysis

The response of structure and nitrogen removal function of the biofilm on submerged macrophytes to high ammonium in constructed wetlands

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Journal of environmental Sciences 2024年第8期142卷 129-141页

作者： Xue Jiang Mengmeng Wang Shunqing Yang Di He Fei Fang Liuyan Yang state key laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China School of resources and environment Anqing Normal UniversityAnqing 246133China

The ammonium exceedance discharge from sewage treatment plants has a great risk to the stable operation of subsequent constructed wetlands(CWs).The effects of high ammonium shocks on submerged macrophytes and epiphytic biofilms on the leaves of submerged macrophytes in CWs were rarely mentioned in previous studies.In this paper,the 16S rRNA sequencing method was used to investigate the variation of the microbial communities in biofilms on the leaves of Vallisneria natans plants while the growth characteristics of V.natans plants were measured at different initial ammonium concentrations.The results demonstrated that the total chlorophyll and soluble sugar synthesis of V.natans plants decreased by 51.45%and 57.16%,respectively,and malondialdehyde content increased threefold after8 days if the initial NH_(4)^(+)-N concentration was more than 5 mg/L.Algal density,bacterial quantity,dissolved oxygen,and pH increased with high ammonium shocks.The average removal efficiencies of total nitrogen and NH_(4)^(+)-N reached 73.26%and 83.94%,respectively.The heat map and relative abundance analysis represented that the relative abundances of phyla Proteobacteria,Cyanobacteria,and Bacteroidetes increased.The numbers of autotrophic nitrifiers and heterotrophic nitrification aerobic denitrification(HNAD)bacteria expanded in biofilms.In particular,HNAD bacteria of Flavobacterium,Hydrogenophaga,Acidovorax,Acinetobacter,Pseudomonas,Aeromonas,and Azospira had higher abundances than autotrophic nitrifiers because there were organic matters secreted from declining leaves of V.natans plants.The analysis of the nitrogen metabolic pathway showed aerobic denitrification was the main nitrogen removal pathway.Thus,the nitrification and denitrification bacterial communities increased in epiphytic biofilms on submerged macrophytes in constructed wetlands while submerged macrophytes declined under ammonium shock loading.

关键词： Ammonium shock loading Biofilm Autotrophic nitrifiers Heterotrophic nitrification aerobic denitrification bacteria Submerged macrophyte

Assessment of tree-ring mercury radial translocation and age effect in Masson pine:Implications for historical atmospheric mercury reconstruction

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Journal of environmental Sciences 2024年第4期138卷 266-276页

作者： Xu Liu Xun Wang Dingyong Wang College of resources and environment Southwest UniversityChongqing 400715China state key laboratory of environmental Geochemistry Institute of GeochemistryChinese Academy of SciencesGuiyang 550081China

The tree ring has been regarded as an emerging archive to reconstruct historical atmospheric mercury(Hg)trends,but with the large knowledge gaps in the reliability.In this study,we comprehensively evaluated the Hg source,radial translocation and age effect of Masson pine(Pinus massoniana)tree ring at Mt.Jinyun in Chongqing,to assess the suitability of such tree ring as the archive of atmospheric Hg.Results showed that distinct variabilities among Masson pine tree-ring Hg concentration profiles.The Hg concentration significantly increased along with stem height(P<0.05),indicating the Hg in tree rings mainly derived from foliage uptake atmospheric Hg.We found a distinct age effect that the tree ring of young trees had the higher Hg concentration.Besides,we used the advection-diffusion model to demonstrate how Hg concentration shifted by the advection or/and diffusion in tree rings.The modeling results showed that the advection induced radial translocation during the young growth period of tree was a plausible mechanism to result in the tree-ring Hg record largely different from the trend of anthropogenic Hg emissions in Chongqing.We finally suggest that in further Hg dendrochemistry,better discarding the tree-ring Hg profile of the young growth period to reduce impacts of the radial translocation and age effect.

关键词： Masson pine Tree-ring mercury Radial translocation Tree age effect

Facet-dependent activation of oxalic acid over hematite nanocrystals under the irradiation of visible light for efficient degradation of pollutants

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Journal of environmental Sciences 2024年第8期142卷 204-214页

作者： Zhixiong Yang Yuan Li Xiaotian Wang Jiaming Li Jiquan Wang Gaoke Zhang Hubei key laboratory of Mineral resources Processing and environment State Key Laboratory of Silicate Materials for ArchitecturesWuhan University of TechnologyWuhan 430070China Hubei Engineering Consulting Co. Ltd.Wuhan 430071China

Naturally occurring hematite has been widely studied in the Fenton-like system for water pollutant remediation due to its abundance and non-toxicity.However,its inadequate catalytic activity results in difficulty in effectively degrading pollutants in the catalytic degradation system that it constitutes.Thus,we constructed a photochemical system composed of hematite with{001}facet of high activity facet and low-cost and non-toxic oxalic acid(OA)for the removal of various types of pollutants.The removal rate for the degradation of metronidazole,tetracycline hydrochloride,Rhodamine B,and hexavalent chromium by hematite nanoplate with the exposed{001}facet activating OA under visible light irradiation was 4.75,2.25,2.33,and 2.74 times than that by the exposed{110}facet,respectively.Density functional theory(DFT)calculation proved that the OA molecule was more easily adsorbed on the{001}facet of hematite than that on the{110}facet,which would favor the formation of the more Fe(Ⅲ)-OA complex and reactive species.In addition,the reactive site of metronidazole for the attraction of radicals was identified on the basis of the DFT calculation on the molecular occupied orbitals,and the possible degradation pathway for metronidazole included carbon chain fracture,hydroxyethyl-cleavage,denitrogenation,and hydroxylation.Thus,this finding may offer a valuable direction in designing an efficient iron-based catalyst based on facet engineering for the improved activity of Fenton-like systems such as OA activation.

关键词： Hematite Facet exposure Oxalic acid activation Fenton-like system Pollutant removal