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Conductive and stable polyphenylene/CNT composite membrane for electrically enhanced membrane fouling mitigation

Frontiers of environmental science & engineering 2024年第1期18卷 35-47页

作者： Huijuan Xie Haiguang Zhang Xu Wang Gaoliang Wei Shuo Chen Xie Quan Key Laboratory of Industrial Ecology and environmental engineering(Ministry of Education) School of Environmental Science and TechnologyDalian University of TechnologyDalian 116024China

Nanocarbon-based conductive membranes, especially carbon nanotube (CNT)-based membranes, have tremendous potential for wastewater treatment and water purification because of their excellent water permeability and selectivity, as well as their electrochemically enhanced performance (e.g., improved antifouling ability). However, it remains challenging to prepare CNT membranes with high structural stability and high electrical conductivity. In this study, a highly electroconductive and structurally stable polyphenylene/CNT (PP/CNT) composite membrane was prepared by electropolymerizing biphenyl on a CNT hollow fiber membrane. The PP/CNT membrane showed 3.4 and 5.0 times higher electrical conductivity than pure CNT and poly(vinyl alcohol)/CNT (PVA/CNT) membranes, respectively. The structural stability of the membrane was superior to that of the pure CNT membrane and comparable to that of the PVA/CNT membrane. The membrane fouling was significantly alleviated under an electrical assistance of −2.0 V, with a flux loss of only 11.7% after 5 h filtration of humic acid, which is significantly lower than those of PP/CNT membranes without electro-assistance (56.8%) and commercial polyvinylidene fluoride (PVDF) membranes (64.1%). Additionally, the rejection of negatively charged pollutants (humic acid and sodium alginate) was improved by the enhanced electrostatic repulsion. After four consecutive filtration-cleaning cycle tests, the flux recovery rate after backwashing reached 97.2%, which was much higher than those of electricity-free PP/CNT membranes (67.0%) and commercial PVDF membranes (61.1%). This study offers insights into the preparation of stable conductive membranes for membrane fouling control in potential water treatment applications.

关键词： Polyphenylene CNTs Membrane Electro-assistance Membrane fouling mitigation

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Enhanced interfacial charge transfer on Bi metal@defective Bi_(2)Sn_(2)O_(7) quantum dots towards improved full-spectrum photocatalysis:A combined experimental and theoretical investigation

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Chinese Chemical Letters 2024年第6期35卷 507-514页

作者： Huizhong Wu Ruiheng Liang Ge Song Zhongzheng Hu Xuyang Zhang Minghua Zhou Tianjin Key Laboratory of environmental Technology for Complex Trans-Media Pollution College of Environmental Science and EngineeringNankai UniversityTianjin 300350China Key Laboratory of Pollution Process and environmental Criteria Ministry of EducationCollege of Environmental Science and EngineeringNankai UniversityTianjin 300350China

To mitigate the water pollution problem by photocatalytic degradation of typical antibiotics of tetracycline(TC),we prepared defective Bi_(2)Sn_(2)O_7(BSO)quantum dots(QDs)with a full spectral response due to Bi metal deposition,using a one-pot hydrothermal method,labeled as Bi@*** optimized Bi@BSOOV showed 73.4% removal of TC in 1 h under irradiation with a 50 W LED lamp in the wavelength band in the visible-near-infrared(vis-NIR)light,a rate that is substantially greater than that of pure BSO(14.7%).The synergistic interaction of Bi metal and oxygen vacancies(OVs)is crucial to boosting photocatalytic *** near-infrared region of the photo-response is extended by the surface plasmon resonance(SPR)effect of Bi metal,enhancing the photocatalytic performance and dramatically raising the efficiency of solar energy *** addition to inducing defect levels in BSO,the OVs also activate the surface adsorbed O_(2) to promote the production of·O_(2)^(-)and ^(1)O_(2).DFT calculations reveal that Bi metal and OVs can mutually tune the charge transfer *** the one hand,Bi metal can act as both a charge transfer bridge and an electron donor to assist charge *** the other hand,OVs-induced defect levels allow electrons that leap to the conduction band(CB)to first leap from the valence band(VB)to the defect levels,notably improving interfacial charge separation and *** concept of design executed in this study for altering the catalyst by introducing both OVs and Bi metal can provide a rational design idea and potential insight for improving the photocatalytic activity for environmental applications.

关键词： Bi metal Bi_(2)Sn_(2)O_7 quantum dots Surface plasmon resonance Oxygen vacancies

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Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao Zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao Sihui Zhan MOE Key Laboratory of Pollution Processes and environmental Criteria/Tianjin Key Laboratory of environmental Remediation and Pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen ***,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major ***,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/*** feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom *** article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting *** article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

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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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Degradation of iopamidol in the permanganate/sulfite process:Evolution of iodine species and effect on the subsequent formation of disinfection by-products

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Journal of environmental sciences 2024年第1期135卷 345-352页

作者： Yimin Lin Hongyu Dong Yating Zhu Gongming Zhou Junlian Qiao Xiaohong Guan State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Department of environmental science School of Ecological and Environmental SciencesEast China Normal UniversityShanghai 200241China

Permanganate/sulfite(Mn(VII)/S(IV))process is a promising pre-oxidation technology for sequestering the emerging organic contaminants in drinking water treatment ***(IPM),a representative of iodinated X-ray contrast media,has been widely detected in water sources and has the risk of forming iodinated disinfection byproducts(I-DBPs)in water treatment *** this study,we investigated the evolution of iodine species during the IPM degradation by the Mn(VII)/S(IV)process and its effect on the subsequent formation of I-DBPs during chlorination at pH 7.0 and *** could be effectively degraded in the Mn(VII)/S(IV)process at environmentally relevant pH(pH 7.0 and 8.0).The results of quenching and competitive oxidation kinetic experiments revealed that SO^(·-)_(4)was the major reactive oxidizing species contributing to the degradation of IPM whereas the contributions of HO·and reactive manganese species were negligible in the Mn(VII)/S(IV)process.I–and IO–3were generated while no HOI was detected during the degradation of IPM in the Mn(VII)/S(IV)*** effects of IPM oxidation by Mn(VII)/S(IV)on the subsequent formation of chlorinated disinfection by-products(Cl-DBPs)during chlorination were related to the category of *** pre-oxidation of IPM by Mn(VII)/S(IV)resulted in the generation of I-DBPs during the disinfection process although no I-DBPs were detected if no pre-oxidation was *** finding of this study suggested that attention should be paid to the toxicity of DBPs when water containing iodinated organic contaminants is treated by Mn(VII)/S(IV)process or other pre-oxidation technologies.

关键词： Permanganate/sulfite Iopamidol Sulfate radical Iodinated disinfection byproducts Pre-oxidation

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Next generation desalination membrane with exceptional chlorine resistance

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science China Chemistry 2024年第11期67卷 3500-3502页

作者： Shihong Lin Xinglin Lu Department of Civil and environmental engineering Vanderbilt University CAS Key Laboratory of Urban Pollutant Conversion Department of Environmental Science and Engineering National Synchrotron Radiation Laboratory University of Science and Technology of China

This highlight draws inspiration from a recent publication in science where Zhang and co-workers [1] from Nanjing University of science and Technology reported a novel multifunctional polyester reverse osmosis(RO) membrane and its application in seawater desalination. This research represents a notable advancement in the field, as polyester membranes may potentially compete with state-of-the-art polyamide RO membranes in the mainstream market.

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Enhancing Direct Electrochemical CO2 Electrolysis by Introducing A-Site Deficiency for the Dual-Phase Pr（Ca）Fe（Ni）O3-δ Cathode

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Energy & environmental Materials 2024年第5期7卷 210-218页

作者： Wanhua Wang Haixia Li Ka-Young Park Taehee Lee Dong Ding Fanglin Chen Department of Mechanical engineering University of South Carolina Energy & environmental science and Technology Idaho National Laboratory

High-temperature CO2electrolysis via solid oxide electrolysis cells (CO2-SOECs) has drawn special attention due to the high energy convention efficiency,fast electrode kinetics,and great potential in carbon ***,the development of cathode materials with high catalytic activity and chemical stability for pure CO2electrolysis is still a great *** this work,A-site cation deficient dual-phase material,namely(Pr0.4Ca0.6)xFe0.8Ni0.2O3-δ（PCFN,x=1,0.95,and 0.9）,has been designed as the fuel electrode for a pure CO2-SOEC,which presents superior electrochemical *** all these compositions,(Pr0.4Ca0.6)0.95Fe0.8Ni0.2O3-δ（PCFN95） exhibited the lowest polarization resistance of 0.458Ωcm2at open-circuit voltage and 800℃.The application of PCFN95 as the cathode in a single cell yields an impressive electrolysis current density of 1.76 A cm-2at 1.5 V and 800℃,which is76%higher than that of single cells with stoichiometric Pr0.4Ca0.6Fe0.8Ni0.2O3-δ（PCFN100） *** effects of A-site deficiency on materials'phase structure and physicochemical properties are also systematically *** an enhancement in electrochemical performance is attributed to the promotion of effective CO2adsorption,as well as the improved electrode kinetics resulting from the A-site deficiency.

关键词： A-site deficiency cathode material CO2 adsorption direct CO2 electrolysis solid oxide electrolysis cells

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Morphology and valence state evolution of Cu:Unraveling the impact on nitric oxide electroreduction

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Journal of Energy Chemistry 2024年第4期91卷 276-286页

作者： Ting Sun Fengyu Gao Ya Wang Honghong Yi Qingjun Yu Shunzheng Zhao Xiaolong Tang School of Energy and environmental engineering University of Science and Technology BeijingBeijing 100083China

Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas ***,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas *** address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable ***(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and ***,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR *** this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth ***,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V *** hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ***,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same *** distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation *** Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by *** findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.

关键词： NORR Ammonia Synthesis Copper Morphology Valence States Mechanism

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Electrochemical filtration for drinking water purification:A review on membrane materials,mechanisms and roles

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Journal of environmental sciences 2024年第7期141卷 102-128页

作者： Yuying Qi Donghao Li Shixuan Zhang Fengxiang Li Tao Hua College of environmental science and engineering Nankai UniversityTianjin 300350China Key Laboratory of Pollution Process and environmental Criteria Ministry of EducationTianjin 300350China Tianjin engineering Center of environmental Diagnosis and Contamination Remediation Tianjin 300350China

Electrochemical filtration can not only enrich low concentrations of pollutants but also produce reactive oxygen species to interact with toxic pollutants with the assistance of a power supply,making it an effective strategy for drinking water *** addition,the application of electrochemical filtration facilitates the reduction of pretreatment procedures and the use of chemicals,which has outstanding potential for maximizing process simplicity and reducing operating costs,enabling the production of safe drinking water in smaller *** recent years,the research on electrochemical filtration has gradually increased,but there has been a lack of attention on its application in the removal of low concentrations of pollutants from low conductivity *** this review,membrane substrates and electrocatalysts used to improve the performance of electrochemical membranes are briefly ***,the application prospects of emerging single-atom catalysts in electrochemical filtration are also ***,several electrochemical advanced oxidation processes coupled with membrane filtration are described,and the related working mechanisms and their advantages and shortcomings used in drinking water purification are ***,the roles of electrochemical filtration in drinking water purification are presented,and the main problems and future perspectives of electrochemical filtration in the removal of low concentration pollutants are discussed.

关键词： Electrochemical filtration Drinking water Conductive membrane Low concentration Electrocatalyst

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Colloid-facilitated release of polybrominated diphenyl ethers at an e-waste recycling site: evidence from undisturbed soil core leaching experiments

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Frontiers of environmental science & engineering 2024年第2期18卷 91-101页

作者： Zebin Huo Mengjun Xi Lianrui Xu Chuanjia Jiang Wei Chen College of environmental science and engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300350China

Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.

关键词： Polybrominated diphenyl ether Colloid-facilitated transport E-waste recycling site Undisturbed soil core Groundwater quality

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