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COF-based membranes for liquid phase separation:Preparation,mechanism and perspective

Journal of environmental sciences 2024年第7期141卷 63-89页

作者： Yujie Zhao He Gu Yilun Zhou CaimeiWen Xiaolu Liu Suhua Wang Zhongshan Chen Hui Yang Xiangke Wang college of environmental science and engineering North China Electric Power UniversityBeijing 102206China School of environmental science and engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Covalent organic frameworks(COFs)are a new kind of crystalline porous materials composed of organic molecules connected by covalent bonds,processes the characteristics of low density,large specific surface area,adjustable pore size and structure,and easy to functionalize,which have been widely used in the field of membrane separation technology.Recently,there are more and more researches focusing on the preparation methods,separation application,and mechanism of COF membranes,which need to be further summarized and compared.In this review,we primarily summarized several conventional preparation methods,such as two-phase interfacial polymerization,in-situ growth on substrate,unidirectional diffusion method,layer-by-layer assembly method,mixed matrix membranes,and so on.The advantages and disadvantages of each method are briefly summarized.The application potential of COF membrane in liquid separation are introduced from four aspects:dyeing wastewater treatment,heavy metal removal,seawater desalination and oil-water separation.Then,the mechanisms including pore structure,hydrophilic/hydrophobic,electrostatic repulsion/attraction and Donnan effect are introduced.For the efficient removal of different kind of pollutions,researchers can select different ligands to construct membranes with specific pore size,hydrophily,salt or organic rejection ability and functional group.The ideas for the design and preparation of COF membranes are introduced.Finally,the future direction and challenges of the next generation of COF membranes in the field of separation are prospected.

关键词： Covalent organic frameworks Membrane materials Liquid phase separation Separation mechanism

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Glutamicibacter nicotianae AT6:A new strain for the efficient biodegradation of tilmicosin

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Journal of environmental sciences 2024年第8期142卷 182-192页

作者： Huijuan Li Hao Zhou Liling Fan Long Meng Yanyun Zhao Lanmei Zhao Bo Wang college of Chemical and Biological engineering Shandong University of Science and TechnologyQingdao 266590China college of Chemistry and Chemical engineering Heze UniversityHeze 274015China college of Safety and environmental engineering Shandong University of Science and TechnologyQingdao 266590China

The degradation of tilmicosin(TLM),a semi-synthetic 16-membered macrolide antibiotic,has been receiving increasing attention.Conventionally,there are three tilmicosin degradation methods,and among them microbial degradation is considered the best due to its high efficiency,eco-friendliness,and low cost.Coincidently,we found a new strain,Glutamicibacter nicotianae sp.AT6,capable of degrading high-concentration TLM at 100 mg/L with a 97%removal efficiency.The role of tryptone was as well investigated,and the results revealed that the loading of tryptone had a significant influence on TLM removals.The toxicity assessment indicated that strain AT6 could efficiently convert TLM into less-toxic substances.Based on the identified intermediates,the degradation of TLM by AT6 processing through two distinct pathways was then proposed.

关键词： Tilmicosin Glutamicibacter nicotianae Biodegradation Degradation pathway Pharmaceutical wastewater

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FeNi Prussian blue analogues on highly graphitized carbon nanosheets as efficient glucose sensors

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Rare Metals 2024年第6期43卷 2730-2738页

作者： Jin-Hang Xue Qiu-Hong Sun Cheng Han Yuan-Dong Yang Shao-Jie Xu Qi-Peng Li Jin-Jie Qian college of Life and environmental science Wenzhou University college of Chemistry and Materials engineering Wenzhou University college of Chemistry and Chemical engineering Zhaotong University

Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and stability.In this study,a straightforward strategy was proposed for synthesizing ultra-thin oxygen-rich graphitized carbon nanosheets（denoted as GCS-O）.These nanosheets are obtained by calcining a topologically two-dimensional indium-based coordination polymer.Subsequently,the growth of FeNi Prussian blue analogue（PBA） on GCS-O effectively introduces active sites and increases the nitrogen content within the carbonaceous matrix.The resulting FeNi-PBA/GCS-O composite exhibits excellent glucose sensing performance with a broad linear range of 1 to 1300μmol·L-1.Meanwhile,it also achieves a high sensitivity of 2496 μA·mmol-1·L·cm-2,a limit of detection of 100nmol·L-1（S/N=3）,and commendable long-term durability.The relatively simple synthesis process,exceptional sensitivity,and satisfactory electrochemical sensing performance of FeNi-PBA/GCS-O open up new directions for biosensor applications.

关键词： Coordination polymer Carbon nanosheet Prussian blue analogue Surface reconstruction Glucose oxidation

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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 plant.Iopamidol(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 system.In 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 8.0.IPM 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)process.The 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 Cl-DBPs.The 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 applied.The 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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Spherical Bi_(2)O_(3)/ATO catalyst with N_(2)pre-reduction electrocatalytic reduction of CO_(2)to formic acid

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Journal of environmental sciences 2024年第6期140卷 331-340页

作者： Junying Yi Yuli Chen Dongze Lai Bihong Lv Xiaomin Wu Guohua Jing Department of environmental science&engineering College of Chemical EngineeringHuaqiao UniversityXiamenFujian 361021China

To achieve carbon neutrality,the Chinese government needs to gain a comprehensive understanding of the sources and drivers of greenhouse gas(GHG)emissions,particularly at the county level.Anji County in eastern China is a typical example of an industrial transformation from quarrying to a low-carbon economy.This study analyzed the decoupling types and structural characteristics of GHG emissions and the driving factors of carbon dioxide(CO_(2))emissions in the Anji from 2006 to 2019,and explored the differences between countylevel and provincial-level or city-level results.It was observed that energy-related activities are the main source of GHG emissions in Anji and that economic development is the driving factor behind the increasing CO_(2)emissions.However,industrial transformation and upgradation coupled with the alternative use of clean energy limit the growth of GHG emissions.This study details the GHG emissions of county during the industrial transformation stage and provides corresponding policy recommendations for county governments.

关键词： N_(2)prereduction CO_(2)electroreduction Bi_(2)O_(3)/ATO catalyst Formate

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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 purification.In 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 installations.In 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 water.In this review,membrane substrates and electrocatalysts used to improve the performance of electrochemical membranes are briefly summarized.Meanwhile,the application prospects of emerging single-atom catalysts in electrochemical filtration are also presented.Thereafter,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 illustrated.Finally,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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Distribution and bioavailability of mercury in size-fractioned atmospheric particles around an ultra-low emission power plant in Southwest China

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Journal of environmental sciences 2024年第4期138卷 141-152页

作者： Wei Zhang Jinjuan Li Hao Qiu Xingqiang Guo Zhijun Fei Yi Xing Deliang Yin college of Resources and environmental engineering Guizhou UniversityGuiyang 550025China college of Resources and environmental engineering Guizhou Institute of TechnologyGuiyang 550003China Key Laboratory of Karst Georesources and Environment(Guizhou University) Ministry of EducationGuiyang 550025China School of Energy and environmental engineering University of Science&Technology BeijingBeijing 100083China

Ultra-low emission(ULE)technology retrofits significantly impact the particulate-bound mercury(Hg)emissions from coal-fired power plants(CFPPs);however,the distribution and bioavailability of Hg in size-fractioned particulate matter(PM)around the ULE-retrofitted CF-PPs are less understood.Here,total Hg and its chemical speciation in TSP(total suspended particles),PM_(10)(aerodynamic particle diameter≤10μm)and PM_(2.5)(aerodynamic particle diameter≤2.5μm)around a ULE-retrofitted CFPP in Guizhou Province were quantified.Atmospheric PM_(2.5)concentration was higher around this ULE-retrofitted CFPP than that in the intra-regional urban cities,and it had higher mass Hg concentration than other sizefractioned PM.Total Hg concentrations in PM had multifarious sources including CFPP,vehicle exhaust and biomass combustion,while they were significantly higher in autumn and winter than those in other seasons(P40%).Mass concentrations of exchangeable,HCl-soluble,elemental,and residual Hg in PM_(2.5)were higher than those in other size-fractioned PM,and were markedly elevated in autumn and winter(P<0.05).In PM_(2.5),HCl-soluble Hg presented a significantly positive relationship with elemental Hg(P<0.05),while residual Hg showed the significantly positive relationships with HCl-soluble Hg and elemental Hg(P<0.01).Overall,these results suggested that atmospheric PM-bound Hg around the ULE-retrofitted CFPP tends to accumulate in finer PM,and has higher bioavailable fractions,while has potential transformation between chemical speciation.

关键词： Size-fractioned particles Mercury Chemical speciation Coal-fired power plant Ultra-low emission

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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 concerns.Hydrolysis kinetics that is of importance for assessing environmental persistence of chemicals remain elusive for MPEs.Herein,kinetics of base-catalyzed and neutral hydrolysis for 18 MPEs with different leaving groups was investigated by density functional theory calculation.Results indicate that MPEs with leaving groups having p Kaof<10 prefer dissociative transition states.MPEs 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 parameters.It was found that p Kaof the leaving groups and electronegativity of the MPEs are key factors determining the hydrolysis kinetics.This 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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Iron-doped Mn-Ce/TiO_2 catalyst for low temperature selective catalytic reduction of NO with NH_3

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Journal of environmental sciences 2010年第9期22卷 1447-1454页

作者： Boxiong Shen ,Ting Liu,Ning Zhao,Xiaoyan Yang,Lidan Deng college of environmental science and engineering,Nankai University,Tianjin 300071,China. college of environmental science and engineering Nankai University Tianjin 300071 China

The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over Fe-Mn-Ce/TiO2 was obviously improved after iron doping compared with that over Mn-Ce/TiO2. Fe-Mn-Ce/TiO2 with the molar ratio of Fe/Ti = 0.1 exhibited the highest activity. The results showed that 96.8% NO conversion was obtained over Fe（0.1）-Mn-Ce/TiO2 at 180~C at a space velocity of 50,000 hr-1. Fe-Mn-Ce/TiO2 exhibited much higher resistance to H2O and SO2 than that of Mn-Ce/TiO2. The properties of the catalysts were characterized using X-ray diffraction （XRD）, N2 adsorption, temperature programmed desorption （NH3-TPD and NOx-TPD）, and X- ray photoelectron spectroscopy （XPS） techniques. BET, NH3-TPD and NOx-TPD results showed that the specific surface area and NH3 and NOx adsorption capacity of the catalysts increased with iron doping. It was known from XPS analysis that iron valence state on the surface of the catalysts were in Fe^3＋ state. The doping of iron enhanced the dispersion and oxidation state of Mn and Ce on the surface of the catalysts. The oxygen concentrations on the surface of the catalysts were found to increase after iron doping. Fe-Mn-Ce/TiO2 represented a promising catalyst for low temperature SCR of NO with NH3 in the presence of H20 and SO2.

关键词： low-temperature SCR Fe-Mn-Ce/TiO2 H2O SO2

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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@BSO-OV.The 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 performance.The 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 utilization.In 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 pathways.On the one hand,Bi metal can act as both a charge transfer bridge and an electron donor to assist charge separation.On 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 transfer.The 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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