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Antibiotic ciprofloxacin removal from aqueous solutions by electrochemically activated persulfate process:Optimization,degradation pathways,and toxicology assessment

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Journal of environmental Sciences 2024年第9期143卷 85-98页

作者： Elif Yakamercan Ahmet Aygün Halis Simsek environmental engineering Department Bursa Technical UniversityBursaTurkey Agricultural and biological engineering Department Purdue UniversityWest LafayetteINUSA

Ciprofloxacin(CIP)is a commonly used antibiotic in the fluoroquinolone group and is widely used in medical and veterinary medicine disciplines to treat bacterial infections.When CIP is discharged into the sewage system,it cannot be removed by a conventional wastewater treatment plant because of its recalcitrant characteristics.In this study,boron-doped diamond anode and persulfate were used to degrade CIP in an aquatic solution by creating an electrochemically activated persulfate(EAP)process.Ironwas added to the system as a coactivator and the process was called EAP+Fe.The effects of independent variables,including pH,Fe^(2+),persulfate concentration,and electrolysis time on the systemwere optimized using the response surface methodology.The results showed that the EAP+Fe process removed 94%of CIP under the following optimum conditions:A pH of 3,persulfate/Fe^(2+)concentration of 0.4 mmol/L,initial CIP concentration 30 mg/L,and electrolysis time of 12.64 min.CIP removal efficiency was increased from 65.10%to 94.35%by adding Fe^(2+)as a transition metal.CIP degradation products,7 pathways,and 78 intermediates of CIP were studied,and three of those intermediates(m/z 298,498,and 505)were reported.The toxicological analysis based on toxicity estimation software results indicated that some degradation products of CIP were toxic to targeted animals,including fathead minnow,Daphnia magna,Tetrahymena pyriformis,and rats.The optimumoperation costswere similar in EAP and EAP+Fe processes,approximately 0.54€/m^(3).

关键词： Ciprofloxacin Response surface methodology Electrochemically activated persulfate Electrooxidation

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An efficient approach for the treatment of radioactive waste perfluoropolyether lubricants via a synergistic effect of thermal catalysis and immobilization

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Journal of environmental Sciences 2024年第2期136卷 512-522页

作者： Xinhang Du Wenhua Tong Xinyu Zhou Jia Luo Yuqiu Liu Yabo Wang Panyu Li Yongkui Zhang Department of Pharmaceutical&biological engineering School of Chemical EngineeringSichuan UniversityChengdu 610065China

Perfluoropolyether(PFPE)lubricants are a kind of high-molecular polymer with many excellent properties.However,the use of PFPEs in the nuclear industry can lead to partial decomposition and carrying radionuclides,resulting in a large amount of radioactive waste PFPE lubricants annually.Moreover,radioactive waste PFPE lubricants are difficult to be effectively treated due to their high stability,the risk of possible leakage of radionuclides,and hypertoxic fluorine-containing by-products.In this study,without any precedent,a strategy of Mn O_(2)-catalyzed decomposition and Na_(2)CO_(3)-immobilized conversion was proposed for PFPE lubricant decomposition and fluorine immobilization simultaneously based on the Lewis acid-base and oxygen vacancies concept.A high fluorine conversion efficiency of 95.4%was achieved.Meanwhile,the mechanism of decomposition suggested that Mn O_(2)mainly provided Lewis acid sites and attacked the(basic)fluorine or oxygen atoms in PFPE molecules.The decomposition of PFPE chains was proceed down and volatile fluorine-containing gas was released by partial electron transfer,intramolecular disproportionation reaction,and unzipping fashion.Subsequently,gas by-products could be further oxidized and then immobilized into fluoride salts by carbonate solid absorbents.Overall,this study provides a simple,safe,and potentially practical strategy for the harmless conversion of refractory fluorinated organic wastes,especially perfluoropolymers.

关键词： Perfluoropolyether lubricants Catalyzed decomposition Fluorine-containing gas Immobilized conversion Fluoride

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The homogenous growth of Co-based coordination compound on graphene nanosheet for high-performance K-organic battery and its reaction mechanism

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Rare Metals 2024年第4期43卷 1622-1634页

作者： Qian-Qian Peng Yi-Ting Wang Shuo Qi Yao Xiao Yong Wang Shuang-Qiang Chen school of environmental and Chemical engineering Shanghai University school of Chemistry and Materials engineering Wenzhou University

Metal coordination compounds（MCCs） are gaining popularity for potassium-ion batteries（PIBs）owing to their tuneable structure,multiple reaction sites,low cost and unique morphology.However,they are generally subjected to intrinsic features of the sluggish ionic diffusion coefficient,low electronic conductivity and slow kinetics.Herein,a new MCC material of cobalt-1,3,5-trioxy-2,4,6-triamino-benzo（Co-TB） coordination compound was synthesized and homogenously grown on the surface of graphene nanosheets（GNS）,forming a Co-TB@GNS composite with enhanced electronic conductivity and flexible capability.Benefiting from the overall enhanced conductivity,high surface area and abundant activated K-storage sites,Co-TB@GNS electrodes have exhibited superior cycling performance with high reversible capacities(312 mAh·g-1after 100 cycles at 100 mA·g-1,224 mAh·g-1after 500 cycles at 1 A·g-1) and better rate performances compared with the pure Co-TB compound when served as PIB's anodes.Furthermore,multiple in-situ measurement techniques have jointly confirmed that the organic functional groups（C=O,C=N and C=C of benzene rings） and Co2+in Co-TB are the main reversible K-storage sites,including in-situ Fourier transform infrared spectroscopy（FTIR） and X-ray diffraction（XRD）,and partial capacity contribution is originated from GNS by the apparent K-storage behavior in the in-situ XRD pattern,proving the possibility of K-storage for metal-organic materials.

关键词： Metal coordination compounds Potassium-ion battery Cobalt coordination compound K-storage mechanism

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Partial aging can counter-intuitively couple with sulfidation to improve the reactive durability of zerovalent iron

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Frontiers of environmental Science & engineering 2024年第2期18卷 1-11页

作者： Yiwei Liu Kaili Gu Jinhua Zhang Jinxiang Li Jieshu Qian Jinyou Shen Xiaohong Guan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China school of Ecological and environmental Sciences East China Normal UniversityShanghai 200241China

Sulfated zero-valent iron(SZVI)has shown promising applications in wastewater treatment.However,the rapid decline in the reactivity of SZVI with time limits its real practice.To mediate this problem,partial aging was proposed to improve the reactive durability of SZVI.Taking Cr(VI)as the target contaminant,we found that the aged ZVI(AZVI)gradually lost reactivity as aging time increased from 0.5 to 2 d.Counter-intuitively,the partially aged SZVI(ASZVI)showed greater reactivity than SZVI when exposed to oxygenated water for a period ranging from 0.5 to 14 d.In addition,the ASZVI with 0.5 d of aging time(ASZVI-0.5)not only maintained reactivity in successive runs but also increased the Cr(VI)removal capacity from 9.1 mg/g by SZVI to 19.1 mg/g by ASZVI-0.5.Correlation analysis further revealed that the electron transfer from the Fe0 core to the shell was mediated by the conductive FeS and FeS2 in the subshell of ASZVI.Meanwhile,the lepidocrocite and magnetite on the surface of ASZVI facilitated Cr(VI)adsorption and subsequent electron transfer for Cr(VI)reduction.Moreover,the iron(hydr)oxide shell could retain the conductive FeS and FeS2 in the subshell,allowing ASZVI to reduce Cr(VI)efficiently and sustainably.In general,partial aging can enhance the reactive durability of ZVI when coupled with sulfidation and this synergistic effect will be beneficial to the application of SZVI-based technology for wastewater treatment.

关键词： Zerovalent iron Sulfidation Partial aging Interface reconstruction Electron transfer

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Constructing core@shell structured photothermal nanosphere with thin carbon layer confined Co-Mn bimetals for pollutant degradation and solar interfacial water evaporation

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Rare Metals 2024年第4期43卷 1686-1701页

作者： Hong-Yang Zhu Meng-Ting Liu Gang Wang Rong-Rong Du Hong-Yao Zhao Hao Lu Shi-Qi Yang Sheng Tang Zeng-Jing Guo Jun Yang Cheng-Zhang Zhu Fu Yang school of environmental and Chemical engineering Jiangsu University of Science and Technology school of Chemistry and Chemical engineering Liaocheng University school of Material Science and engineering Jiangsu University of Science and Technology school of environmental Science and engineering Nanjing Tech University

Photothermal material applied in environmental governance has attracted growing attention.By combining the Stober method and dopamine-triggered coating strategy,Co-Mn precursor was in situ incorporated into the poly dopamine（PDA） layer over the surface of silica cores.Afterwards,a unique photothermal nanosphere with SiO2core and thin carbon layer and dual Co-Mn oxides shell was allowed to form by sequential heat treatment in the inert atmosphere（SiO2@CoMn/C）.The bimetallic fraction of Co/Mn in the carbon layer and post-treatment calcination temperature was comprehensively tuned to optimize the peroxymonosulfate（PMS） activation performance of the catalyst.The state of bimetallic species was studied including their physical distribution,chemical valence,and interplay by various characterizations.Impressively,Co oxides appear as dominant monodispersed nanoparticles（～ 10 nm）,while Mn with cluster-like morphology is observed to uniformly distribute over thin-layer carbon and adhered to the surface of SiO2nanospheres（～ 250 nm）.The calcined temperature could tune the oxidized state of Co species,leading to the optimization of the catalytic performance of introduced dual metal species.As a result,this obtained optimal catalyst integrated the advantages of exposed bimetallic CoMn species and N-doped thin carbon to deliver excellent catalytic PMS activation performance and photothermal synergetic catalytic mineralization ability for diversiform pollutants.Further reactions condition controls and anion interference studies were conducted to identify the adaptability of the optimal catalyst.Moreover,the application of solar-driven interfacial water evaporation using optimal SiO2@Co3Mn1/C-600 catalyst was explored,showing a high water evaporation rate of 1.48 kg·m-2·h-1and an efficiency of 95.2%,further revealing a comprehensive governance functionality of obtained material in the complex pollution condition.

关键词： Photothermal Peroxymonosulfate (PMS) activation Bimetallic synergy Water evaporation Advanced oxidation process

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Study on the mechanism and reaction characteristics of metal-supported phosphogypsum as oxygen carrier in a chemical looping gasification application

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Journal of environmental Sciences 2024年第4期138卷 428-438页

作者： Jing Yang Yujie Ren Shuoyu Chen Jinsuo Lu school of environmental and Municipal engineering Xi’an University of Architecture and TechnologyXi’an 710055China

This study aimed to explore the chemical looping gasification(CLG)reaction characteristics of the metal-supported composite phosphogypsum(PG)oxygen carriers(OCs)and the thermodynamic mechanism.The FactSage 7.1 thermodynamic simulation was used to explore the oxygen release and H_(2)S removal mechanisms.The experimental results showed that the syngas yield of CLG with PG-CuFe_(2)O_(4)was more than that with PG-Fe_(2)O_(3)20/CuO40 or PG-Fe_(2)O_(3)30/CuO30 OC at 1023 K when the water vapor content was 0.3.Furthermore,the maximum syngas yield of the CO selectivity was 70.3% and of the CO_(2)selectivity was 23.8%.The H_(2)/CO value was 0.78,and the highest carbon conversion efficiency was 91.9% in PG-CuFe_(2)O_(4)at the gasification temperature of 1073 K.The metal-supported PG composite oxygen carrier was proved not only as an oxygen carrier to participate in the preparation of syngas but also as a catalyst to catalyze coal gasification reactions.Furthermore,both the experimental results and FactSage 7.1 thermodynamic analysis revealed that the trapping mechanism of H_(2)S by composite OCs was as follows:CuO first lost lattice oxygen as an oxygen carrier to generate Cu_(2)O,which,in turn,reacted with H_(2)S to generate Cu_(2)S.This study provided efficient guidance and reference for OC design in CLG.

关键词： Metal-supported composite phosphogypsum Reaction characteristics Thermodynamic mechanism Chemical looping gasification

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Proteomics Study of Benzene Metabolite Hydroquinone Induced Hematotoxicity in K562 Cells

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Biomedical and environmental Sciences 2024年第4期37卷 341-353页

作者： JIN Yi Shan YI Zong Chun ZHANG Yu Jing RONG Long YU Chun Hong school of biological Science and Medical engineering Beihang UniversityBeijing 100191China school of engineering Medicine Beihang UniversityBeijing 100191China

Objective Hydroquinone(HQ),one of the phenolic metabolites of benzene,is widely recognized as an important participant in benzene-induced hematotoxicity.However,there are few relevant proteomics in HQ-induced hematotoxicity and the mechanism hasn’t been fully understood yet.Methods In this study,we treated K562 cells with 40μmol/L HQ for 72 h,examined and validated protein expression changes by Label-free proteomic analysis and Parallel reaction monitoring(PRM),and performed bioinformatics analysis to identify interaction networks.Results One hundred and eighty-seven upregulated differentially expressed proteins(DEPs)and 279 downregulated DEPs were identified in HQ-exposed K562 cells,which were involved in neutrophilmediated immunity,blood microparticle,and other GO terms,as well as the lysosome,metabolic,cell cycle,and cellular senescence-related pathways.Focusing on the 23 DEGs and 5 DEPs in erythroid differentiation-related pathways,we constructed the network of protein interactions and determined 6 DEPs(STAT1,STAT3,CASP3,KIT,STAT5B,and VEGFA)as main hub proteins with the most interactions,among which STATs made a central impact and may be potential biomarkers of HQ-induced hematotoxicity.Conclusion Our work reinforced the use of proteomics and bioinformatic approaches to advance knowledge on molecular mechanisms of HQ-induced hematotoxicity at the protein level and provide a valuable basis for further clarification.

关键词： Hydroquinone Proteomics Hematotoxicity K562 cells

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Simultaneous purification of minor components in natural products using twin-column recycling chromatography with a step solvent gradient

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Chinese Journal of Chemical engineering 2024年第5期69卷 212-219页

作者： Guangxia Jin Yuxue Wu Feng Wei school of biological and Chemical engineering NingboTech UniversityNingbo 315100China

The isolation of minor components from complex natural product matrices presents a significant challenge in the field of purification science due to their low concentrations and the presence of structurally similar compounds.This study introduces an optimized twin-column recycling chromatography method for the efficient and simultaneous purification of these elusive constituents.By introducing water at a small flowing rate between the twin columns,a step solvent gradient is created,by which the leading edge of concentration band would migrate at a slower rate than the trailing edge as it flowing from the upstream to downstream column.Hence,the band broadening is counterbalanced,resulting in an enrichment effect for those minor components in separation process.Herein,two target substances,which showed similar peak position in high performance liquid chromatography(HPLC)and did not exceed 1.8%in crude paclitaxel were selected as target compounds for separation.By using the twin-column recycling chromatography with a step solvent gradient,a successful purification was achieved in getting the two with the purity almost 100%.We suggest this method is suitable for the separation of most components in natural produces,which shows higher precision and recovery rate compared with the common lab-operated separation ways for natural products(thin-layer chromatography and prep-HPLC).

关键词： Solvent gradient Twin-column recycling chromatography Purification Minor component Natural products

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

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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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Self-templating synthesis of biomass-based porous carbon nanotubes for energy storage and catalytic degradation applications

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Green Energy & Environment 2024年第3期9卷 584-595页

作者： Manman Xu Shiqi Fu Yukai Wen Wei Li Qiongfang Zhuo Haida Zhu Zhikeng Zheng Yuwen Chen Anqi Wang Kai Yan Research Centre for Eco-environmental engineering School of Environment and Civil EngineeringDongguan University of TechnologyDongguan523808China school of environmental Science and engineering Sun Yat-sen UniversityGuangzhou510275China

Dwindling energy sources and a worsening environment are huge global problems,and biomass wastes are an under-exploited source of material for both energy and material generation.Herein,self-template decoction dregs of Ganoderma lucidum-derived porous carbon nanotubes(ST-DDLGCs)were synthesized via a facile and scalable strategy in response to these challenges.ST-DDLGCs exhibited a large surface area(1731.51 m^(2)g^(-1))and high pore volume(0.76 cm^(3)g^(-1)),due to the interlacing tubular structures of precursors and extra-hierarchical porous structures on tube walls.In the ST-DDLGC/PMS system,the degradation efficiency of capecitabine(CAP)reached~97.3%within 120 min.Moreover,ST-DDLGCs displayed high catalytic activity over a wide pH range of 3–9,and strong anti-interference to these typical and ubiquitous anions in wastewater and natural water bodies(i.e.,H_(2)PO_(4)^(-),NO_(3)^(-),Cl^(-) and HCO_(3)^(-)),in which a ^(1)O_(2)-dominated oxidation was identified and non-radical mechanisms were deduced.Additionally,ST-DDLGC-based coin-type symmetrical supercapacitors exhibited outstanding electrochemical performance,with specific capacitances of up to 328.1 F g^(-1)at 0.5 A g^(-1),and cycling stability of up to 98.6%after 10,000 cycles at a current density of 2 A g^(-1).The superior properties of ST-DDLGCs could be attributed to the unique porous tubular structure,which facilitated mass transfer and presented numerous active sites.The results highlight ST-DDLGCs as a potential candidate for constructing inexpensive and advanced environmentally functional materials and energy storage devices.

关键词： Ganoderma lucidum residue Porous carbon nanotubes Self-template method Wastewater treatment Supercapacitor electrode

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