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Insights into the mechanism of multiple Cu-doped Co Fe_(2)O_(4)nanocatalyst activated peroxymonosulfate for efficient degradation of Rhodamine B

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Journal of Environmental Sciences 2024年第3期137卷 382-394页

作者： Yuanmin Mo Xiaoping Zhang School of Environment&Energy South China University of TechnologyGuangzhou Higher Education Mega CentreGuangzhou 510006China The Key Laboratory of pollution control and Ecosystem Restoration in Industry Clusters of Ministry of Education Guangzhou 510006China Guangdong Provincial Key Laboratory of Solid Wastes pollution control and Recycling Guangzhou 510006China Guangdong Provincial Engineering and technology research center for Environmental Risk Prevention and Emergency Disposal Guangzhou 510006China

The multiple metal catalyst as a promising nanomaterial has shown excellent activity in the peroxymonosulfate(PMS)activation for pollutant ***,the role of special sites and in-depth understanding of the PMS activation mechanism are not fully *** this study,a Cu-doped CoFe_(2)O_(4)nanocatalyst(0.5CCF)was synthesized by a sol-gel and calcination method,and used for PMS activation to remove Rhodamine B(RhB).The results showed that the Cu doping obviously enhanced the catalytic performance of CoFe_(2)O_(4),with 99.70%of RhB removed by 0.5CCF while 74.91%in the CoFe_(2)O_(4)within 15 *** on the X-ray photoelectron spectroscopy and electrochemical analysis,this could be ascribed to the more low valence of Co and Fe species generated on the 0.5CCF and faster electron transfers occurred in the 0.5CCF due to the Cu *** addition,Cu doping could provide more reaction sites for the 0.5CCF to activate PMS for RhB *** metal species and the surface hydroxyl were the reaction sites of PMS activation,and the surface hydroxyl played an important role in surface-bound reactive species *** the PMS activation,the Cu not only activated PMS to produce reactive oxygen species(ROS),but also regenerated Co^(2+)and Fe^(2+)to accelerate the PMS *** non-radical of ^(1)O_(2)was the main ROS with a 99.35%of contribution rate,and the SO_(5)^(·–)self-reaction was its major *** study provides a new insight to enhance the PMS activation performance of multiple metal catalysts by Cu doping in wastewater treatment.

关键词： Cu-doped CoFe_(2)O_(4)nanocatalyst PMS activation Mechanism Rhodamine B removal

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Asymmetric radical allylation of β-keto esters with vinyl cyclopropanes by dual photoredox/nickel catalysis

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Science China Chemistry 2024年第11期67卷 3807-3816页

作者： Wen-Yuan Qu Xue-Song Zhou Wen-Jing Xiao Jia-Rong Chen Engineering research center of Photoenergy Utilization for pollution control and Carbon Reduction Ministry of EducationCollege of Chemistry Central China Normal University Wuhan Institute of Photochemistry and technology Key Laboratory of Organo-Pharmaceutical Chemistry of Jiangxi Province Gannan Normal University

Radical-involved allylation reactions have emerged as a powerful platform for construction of carbon-carbon and carbonheteroatom bonds, facilitating the strategic incorporation of diverse allyl moieties. Nevertheless, this burgeoning field still faces ongoing challenges, including limitations of radical precursors and coupling partners, and difficulties in achieving enantiocontrol. Herein, we report for the first time a highly enantioselective radical allylation involving β-keto esters with vinyl cyclopropanes utilizing a synergistic dual photoredox/nickel catalysis under visible light irradiation. The mild and redox-neutral catalytic protocol demonstrates an extensive substrate compatibility and good functional tolerance, providing access to enantioenriched β-keto esters featuring quaternary α-stereocenter with good yields and high enantioselectivities. Preliminary mechanistic studies have uncovered that the success of the reaction hinges on the dual roles of nickel catalyst, including in situ formation of photoredox sensitive substrate/Ni complex and the ensuing asymmetric radical addition step.

关键词： asymmetric allylation photoredox catalysis radical addition nickel catalysis β-keto esters vinyl cyclopropanes

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A review of CFD simulation in pressure driven membrane with fouling model and anti-fouling strategy

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Frontiers of Environmental Science & Engineering 2024年第8期18卷 1-29页

作者： Shiyong Miao Jiaying Ma Xuefei Zhou Yalei Zhang Huaqiang Chu State Key Laboratory of pollution control and Resource Reuse Tongji UniversityShanghai 200092China Shanghai Institute of pollution control and Ecological Security Tongji UniversityShanghai 200092China

Pressure-driven membrane filtration systems are widely utilized in wastewater treatment,desalination,and water reclamation and have received extensive attention from *** fluid dynamics(CFD)offers a convenient approach for conducting mechanistic studies of flow and mass transfer characteristics in pressure-driven *** a signature phenomenon in membrane systems,the concentration polarization that accompanies the permeation process is a key factor in membrane performance degradation and membrane fouling *** fouling models(scaling,biofouling and colloidal particle fouling)based on CFD theory have been constructed,and considerable research has been *** representative antifouling strategies with special simulation methods,including patterned membranes,vibration membranes,rotation membranes,and pulsatile flows,have also been *** studies should focus on refining fouling models while considering local hydrodynamic characteristics;experimental observation tools focusing on the internal structure of inhomogeneous fouling layers;techno-economic model of antifouling strategies such as vibrational,rotational and pulsatile flows;and unfavorable hydraulic phenomena induced by rapidly changing flows in simulations.

关键词： Computational fluid dynamics Membrane Fouling model Concentration polarization

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Prediction model on hydrolysis kinetics of phthalate monoester:A density functional theory study

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Journal of Environmental Sciences 2024年第1期135卷 51-58页

作者： Tong Xu Jingwen Chen Deming Xia Weihao Tang Jiansheng Cui Chun Liu Shuangjiang Li College of Environmental Science and Engineering Hebei University of Science and TechnologyShijiazhuang 050000China Key Laboratory of Industrial Ecology and Environmental Engineering(Ministry of Education) School of Environmental Science and TechnologyDalian University of TechnologyDalian 116024China National-Regional Joint Engineering research center for Soil pollution control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China

As primary degradation products of phthalate esters,phthalate monoesters(MPEs)have been widely detected in various aquatic environments and drawn growing toxicological *** kinetics that is of importance for assessing environmental persistence of chemicals remain elusive for ***,kinetics of base-catalyzed and neutral hydrolysis for 18 MPEs with different leaving groups was investigated by density functional theory *** indicate that MPEs with leaving groups having p Kaof<10 prefer dissociative transition *** are more persistent than their parents,and their hydrolysis half-lives were calculated to vary from 3.4 min to 79.2 years(p H=7–9).A quantitative structure-activity relationship model was developed for predicting the hydrolysis kinetics *** was found that p Kaof the leaving groups and electronegativity of the MPEs are key factors determining the hydrolysis *** work may lay a theoretical foundation for better understanding the chemical process that governs MPE persistence in aquatic environments.

关键词： Phthalate monoesters Phthalate esters Hydrolysis Density functional theory Quantitative structure-activity relationship

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Predicting microbial extracellular electron transfer activity in paddy soils with soil physicochemical properties using machine learning

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Science China(Technological Sciences) 2024年第1期67卷 259-270页

作者： OU JiaJun LUO XiaoShan LIU JunYang HUANG LinYan ZHOU LiHua YUAN Yong School of Automation Guangdong University of TechnologyGuangzhou 510006China Guangdong Key Laboratory of Environmental Catalysis and Health Risk control Guangzhou Key Laboratory Environmental Catalysis and Pollution ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China School of Biomedical and Pharmaceutical Sciences Guangdong University of TechnologyGuangzhou 510006China

Soil extracellular electron transfer(EET)is a pivotal biological process within the realm of ***,EET suffers from a lack of predictive ***,an intricately crafted machine learning model has been developed for the purpose of predicting soil EET by using the physicochemical properties of soil as independent input variables and the EET capabilities in terms of current density(j_(max))and Coulombic charge(C_(out))as dependent output *** autoencoder ensemble stacking(AES)model was developed to address the aforementioned issue by integrating support vector machine,multilayer perceptron,extreme gradient boosting,and light gradient boosting machine algorithms as the stacking *** 10-fold crossvalidation,the AES model exhibited notable improvements in predicting j_(max)and C_(out),with average test R^(2)values of 0.83 and 0.84,respectively,surpassing those of single machine learning(ML)models and the basic ensemble *** utilizing partial correlation plots(PDPs),Shapley Additive explanations(SHAP)values,and SHAP decision plots,we quantitatively explained the impact and contribution of the input molecules on the AES model’s predictions of j_(max)and C_(out).In the context of the SHAP method for the AES model,total carbon(TC)was identified as the most correlated descriptor for j_(max),while total organic carbon(TOC)stood out as the most relevant descriptor for C_(out).In the prediction tasks of j_(max)and C_(out)within the AES model,employing a multitask ML approach allowed the model to benefit from the shared information of input variables,thereby enhancing its overall *** study provides a feasible tool for the prediction of soil EET from soil physiochemical properties and an advanced understanding of the relationship between soil physiochemical properties and EET capability.

关键词： extracellular electron transfer paddy soil machine learning prediction autoencoder ensemble stacking model

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Progress and challenges of electrolyte modulation in aqueous zinc-ion batteries

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Rare Metals 2024年第7期43卷 2940-2967页

作者： Qi-Hang Yang Lu-Fei Wang Xiao-Yu Wang Meng-Meng Zhen Tianjin Key Laboratory of Clean Energy and pollution control School of Energy and Environmental EngineeringHebei University of TechnologyTianjin 300071China

As a new type of green battery system,aqueous zinc-ion batteries(AZIBs)have gradually become a research hotspot due to their low cost,high safety,excellent stability,high theoretical capacity(820 mAh·g^(-1))of zinc anode,and low redox potential(-0.76 V *** hydrogen electrode(SHE)).AZIBs have been expected to be an alternative to lithium-ion batteries for large-scale commercial energy storage ***,they are facing thorny issues such as degradation of cycling performance,zinc dendrites,and side *** the same time,these problems cause short cycling life of batteries,thus severely limiting their commercial *** recent years,many more researches have been conducted on the modification of anode and cathode materials of AZIBs,but there is a lack of in-depth discussion on the characteristics and mechanism of electrolyte *** this review,we will make a systematic summary of the current problems with two electrodes in AZIBs,as well as the types and functions of electrolyte ***,we further systematically describe the modulation mechanism of electrolyte additives in the performance of the cathode and *** prospects and development directions of additive modulation strategies for AZIBs electrolytes are prospected.

关键词： Electrolyte additives Aqueous zinc-ion batteries Zinc anode protection Cathode chemistry

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Alcohothermal synthesis of sulfidated zero-valent iron for enhanced Cr(Ⅵ)removal

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Chinese Chemical Letters 2024年第7期35卷 192-195页

作者： Zhongsen Wang Lijun Qiu Yunhua Huang Meng Zhang Xi Cai Fanyu Wang Yang Lin Yanbiao Shi Xiao Liu Engineering research center of Photoenergy Utilization for pollution control and Carbon Reduction of Ministry of Education College of ChemistryCentral China Normal UniversityWuhan 430079China

Sulfidation of zero-valent iron(ZVI)has attracted broad attention in recent years for improving the sequestration of contaminants from ***,sulfidated ZVI(S-ZVI)is mostly synthesized in the aqueous phase,which usually causes the formation of a thick iron oxide layer on the ZVI surface and hinders the efficient electron transfer to the *** this study,an alcohothermal strategy was employed for S-ZVI synthesis by the one-step reaction of iron powder with elemental *** is found that ferrous sulfide(FeS)with high purity and fine crystallization was formed on the ZVI surface,which is extremely favorable for electron ***(Ⅵ)removal experiments confirm that the rate constant of SZVI synthesized by the alcohothermal method was 267.1-and 5.4-fold higher than those of un-sulfidated ZVI and aqueous-phase synthesized S-ZVI,*** characterizations proved that Cr(Ⅵ)was reduced and co-precipitated on S-ZVI in the form of a Fe(Ⅲ)/Cr(Ⅲ)/Cr(Ⅵ)composite,suggesting its environmental benignancy.

关键词： Zero-valent iron Sulfidation Alcohothermal method Cr(Ⅵ)removal

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Underestimated benefits of NO_(x) control in reducing SNA and O_(3) based on missing heterogeneous HONO sources

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Frontiers of Environmental Science & Engineering 2024年第3期18卷 57-67页

作者： Shuping Zhang Haotian Zheng Jun Liu Yao Shi Tianzeng Chen Chaoyang Xue Fenfen Zhang Yueqi Jiang Xiangping Zhang Shovan Kumar Sahu Biwu Chu Jia Xing State Key Joint Laboratory of Environment Simulation and pollution control School of EnvironmentTsinghua UniversityBeijing 100084China China Academy of Civil Aviation Science and technology Beijing 100028China State Key Joint Laboratory of Environment Simulation and pollution control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Yellow River Institute of Hydraulic research Zhengzhou 450003China Centre for Climate research Singapore Meteorological Service SingaporeSingapore 537054Singapore

Substantial NO_(x) emission mitigation is crucial for the synergistic reduction of particulate matter and ozone(O_(3))pollution in *** traditional air quality model does not consider heterogeneous HONO chemistry,leading to uncertainties in estimating the benefits of NO_(x) *** studies have shown that the parameterization of heterogeneous HONO formation increases both the simulated value of sulfate–nitrate–ammonium(SNA)and that of O_(3),thus adding the heterogeneous reactions of HONO into air quality models inevitably leads to changes in the estimated benefits of NO_(x) *** we investigated the changes in SNA and O_(3)concentrations from NO_(x) emission reduction before and after adding heterogeneous HONO reactions in the Community Multi-Scale air Quality(CMAQ)*** heterogeneous HONO reactions in the simulation improved the benefits of NO_(x) reduction in terms of SNA control in *** 80%NO_(x) reduction,the reduction in SNA increased from 36.9%without considering heterogeneous HONO reactions to 42.8%with heterogeneous HONO *** reduction in the maximum daily 8h average(MDA8)O_(3)in summer caused by NO_(x) reduction increased slightly from 4.7%to 5.2%after adding heterogeneous HONO *** results in this study highlight the enhanced effectiveness of NO_(x) controls for the reduction of SNA and O_(3)after considering heterogeneous HONO formation in a complex chemical ambient,demonstrating the importance of NO_(x) controls in reducing PM2.5 and O_(3)pollution in China.

关键词： Heterogeneous HONO NO_(x) reduction PM_(2.5) O_(3)

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Dynamic coupling of ferrihydrite transformation and associated arsenic desorption/redistribution mediated by sulfate-reducing bacteria

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Journal of Environmental Sciences 2024年第1期135卷 39-50页

作者： Wenjing Zhou Huiyan Zhu Shiwen Hu Bowei Zhang Kun Gao Zhi Dang Chongxuan Liu State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater pollution control School of Environmental Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055China The Key Lab of pollution control and Ecosystem Restoration in Industry Clusters Ministry of EducationSouth China University of TechnologyGuangzhou 510006China

Sulfate-reducing bacteria play an important role in the geochemistry of iron(oxyhydr)oxide and arsenic(As)in natural environments;however,the associated reaction processes are yet to be fully *** this study,batch experiments coupled with geochemical,spectroscopic,microscopic,and thermodynamic analyses were conducted to investigate the dynamic coupling of ferrihydrite transformation and the associated As desorption/redistribution mediated by Desulfovibrio vulgaris(***).The results indicated that *** could induce ferrihydrite transformation via S^(2-)-driven and direct reduction *** the absence of SO_(4)^(2-),*** directly reduced ferrihydrite,and As desorption and re-sorption occurred simultaneously during the partial transformation of ferrihydrite to *** increase in SO_(4)^(2-)loading promoted the S^(2-)-driven reduction of ferrihydrite and accelerated the subsequent mineralogical *** the low and medium SO_(4)^(2-)treatments,ferrihydrite was completely transformed to a mixture of magnetite and mackinawite,which increased the fraction of As in the residual phase and stabilized *** the high SO_(4)^(2-)treatment,although the replacement of ferrihydrite by only mackinawite also increased the fraction of As in the residual phase,22.1%of the total As was released into the solution due to the poor adsorption affinity of As to mackinawite and the conversion of As^(5+)to As^(3+).The mechanisms of ferrihydrite reduction,mineralogy transformation,and As mobilization and redistribution mediated by sulfate-reducing bacteria are closely related to the surrounding SO_(4)^(2-)*** results advance our understanding of the biogeochemical behavior of Fe,S,and As,and are helpful for the risk assessment and remediation of As contamination.

关键词： Sulfate-reducing bacteria Arsenic Ferrihydrite Transformation Redistribution

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Ferrihydrite transformation impacted by coprecipitation of lignin:Inhibition or facilitation?

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Journal of Environmental Sciences 2024年第5期139卷 23-33页

作者： Lin Liu Zhihui Yang Weichun Yang Wen Jiang Qi Liao Mengying Si Feiping Zhao School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering research center for control&Treatment of Heavy Metal pollution(CNERC-CTHMP) Changsha 410083China

Lignin is a common soil organic matter that is present in soils,but its effect on the transformation of ferrihydrite(Fh)remains *** matter is generally assumed to inhibit Fh ***,lignin can reduce Fh to Fe(Ⅱ),in which Fe(Ⅱ)-catalyzed Fh transformation ***,the effects of lignin on Fh transformation were investigated at 75℃ as a function of the lignin/Fh mass ratio(0-0.2),pH(4-8)and aging time(0-96 hr).The results of Fh-lignin samples(mass ratios=0.1)aged at different pH values showed that for Fh-lignin the time of Fh transformation into secondary crystalline minerals was significantly shortened at pH 6 when compared with pure Fh,and the Fe(Ⅱ)-accelerated transformation of Fh was strongly dependent on *** pH 6,at low lignin/Fh mass ratios(0.05-0.1),the time of secondary mineral formation decreased with increasing lignin *** high lignosulfonate-content material(lignin:Fh=0.2),Fh did not transform into secondary minerals,indicating that lignin content plays a major role in Fh *** addition,lignin affected the pathway of Fh transformation by inhibiting goethite formation and facilitating hematite *** effect of coprecipitation of lignin on Fh transformation should be useful in understanding the complex iron and carbon cycles in a soil environment.

关键词： Ferrihydrite transformation Lignin Hematite Goethite Fe(Ⅱ)-catalyzed Reactive Fe(Ⅲ)species

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