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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

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Black titanium dioxide nanomaterials for photocatalytic removal of pollutants:A review

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Journal of Materials Science & Technology 2022年第17期112卷 239-262页

作者： Ying Liang Guohe Huang Xiaying Xin Yao Yao Yongping Li Jianan Yin Xiang Li Yuwei Wu Sichen Gao State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentBeijing Normal UniversityBeijing 100875China State Key Joint Laboratory of Environmental Simulation and Pollution Control China-Canada Center for EnergyEnvironment and Ecology ResearchUR-BNUSchool of EnvironmentBeijing Normal UniversityBeijing 100875China Department of Environmental Systems Engineering University of ReginaReginaSKS4S 0A2Canada State Key Laboratory of Marine Pollution(SKLMP) City University of Hong KongKowloonHong Kong SARChina Faculty of Engineering and Applied Science University of ReginaReginaSaskatchewanS4S 0A2Canada

Semiconductor photocatalysis is one of the most widely used environment-friendly technologies for removing various contaminants.As a well-developed photocatalyst,titanium dioxide(TiO_(2))still has limits in its wide bandgap and rapid recombination rate of photogenerated charge carriers.Recently,black TiO_(2)appears as a strong candidate in the improvement of sunlight harvesting,because of its excellent absorption capacity and utilization of solar radiation.Despite extensive applications in both environmental and energy fields,the use of black TiO_(2)as a photocatalyst in Pollutant removal is ambiguous.The primary objective of the review is to comprehensively evaluate the applications of black TiO_(2)in photocatalytic removal of contaminants,including conventional organic contaminants,emerging contaminants,microbes,and heavy metals.The basic properties,photocatalytic mechanism,and synthesis of black TiO_(2)have been summarized and analyzed.Moreover,the stability and recoverability of black TiO_(2)have also been discussed.Finally,the perspectives of the application of black TiO_(2)in Pollutant removal have been further discussed.

关键词： Photocatalysis Back TiO_(2) Ti^(3+)self-doping Nanomaterials Pollutant removal

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Immobilization of laccase on organic–inorganic nanocomposites and its application in the removal of phenolic pollutants

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Frontiers of Chemical Science and Engineering 2023年第7期17卷 867-879页

作者： Wei Zhang Runtang Liu Xu Yang Binbin Nian Yi Hu State Key Laboratory of Materials-Oriented Chemical Engineering School of Pharmaceutical SciencesNanjing Tech UniversityNanjing 210009China

Polydopamine-functionalized nanosilica was synthesized using an inexpensive and easily obtainable raw material,mild reaction conditions,and simple operation.Subsequently,a flexible spacer arm was introduced by using dialdehyde starch as a cross-linking agent to bind with laccase.A high loading amount(77.8 mg∙g^(‒1))and activity retention(75.5%)could be achieved under the optimum immobilization conditions.Thermodynamic parameters showed that the immobilized laccase had a lower thermal deactivation rate constant and longer half-life.The enhancement of thermodynamic parameters indicated that the immobilized laccase had better thermal stability than free laccase.The residual activity of immobilized laccase remained at about 50.0%after 30 days,which was 4.0 times that of free laccase.Immobilized laccase demonstrated excellent removal of phenolic pollutants(2,4-dichlorophenol,bisphenol A,phenol,and 4-chlorophenol)and perfect reusability with 70% removal efficiency retention for 2,4-dichlorophenol after seven cycles.These results suggested that immobilized laccase possessed great reusability,improved thermal stability,and excellent storage stability.Organic–inorganic nanomaterials have a good application prospect for laccase immobilization,and the immobilized laccase of this work may provide a practical application for the removal of phenolic pollutants.

关键词： polydopamine Pollutant removal thermodynamic phenolic pollutants immobilized laccase

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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions

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Journal of Energy Chemistry 2024年第5期92卷 459-483页

作者： Xinying Zhao Yuzhuo Jiang Mengfan Wang Yunfei Huan Qiyang Cheng Yanzheng He Tao Qian Chenglin Yan Collaborative Innovation Center of Suzhou Nano Science and Technology College of EnergySoochow UniversitySuzhou 215006JiangsuChina School of Chemistry and Chemical Engineering Nantong UniversityNantong 226019JiangsuChina School of Petrochemical Engineering Changzhou UniversityChangzhou 213164JiangsuChina

Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.

关键词： Electrocatalytic nitrate reduction Electrocatalytic nitrite reduction Ammonia synthesis Pollutant removal Electrosynthesis

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Enhanced removal of Phenols by MIZ-Cu Nanozyme Exhibiting Laccase-like Activity and Broader Adaptability to Temperature and pH Conditions

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Chemical Research in Chinese Universities 2023年第6期39卷 1111-1118页

作者： WANG Yunlong SUN Yue WANG Le ZHANG Hao HU Jiakang LI Yongxin Key Lab of Groundwater Resources and Environment of Ministry of Education Key Lab of Water Resources and Aquatic Environment of Jilin ProvinceCollege of New Energy and EnvironmentJilin UniversityChangchun 130021P.R.China

Phenolic compounds,classified as persistent organic pollutants,pose a significant threat to both human health and environmental safety.Therefore,the efficient removal of phenolic substances from water is of paramount importance.Laccase,a multicopper oxidase,is commonly utilized for the efficient removal of phenolic contaminants from water due to its highly effective catalytic activity towards phenolic compounds.However,natural laccase exhibits certain limitations that impede its practical implementation in industrial settings,including a restricted pH activity range,diminished enzymatic efficacy at elevated temperatures,and substantial cost implications.In this work,we prepared a nanozyme(MIZ-Cu,MIZ:2-methylimidazole)with laccase-like activity by coordinating 2-methylimidazole and copper.This nanozyme overcomes the deactivation issues observed in natural laccase under high temperature and alkaline conditions.The catalytic activity of the MIZ-Cu towards phenolic compounds surpasses that of natural laccase across a wide range of temperature and pH conditions.Under pH=9,80℃,and 500 mmol/L NaCl conditions,the removal rate of four phenols(catechol,hydroquinone,resorcinol,and phloroglucinol)by MIZ-Cu was much higher than that of natural laccase.The results also demonstrate exceptional removal rates in natural aquatic environments,thereby presenting a promising approach for the treatment of phenol-containing wastewater originating from industrial facilities.

关键词： Nanozyme Laccase Phenol Pollutant removal Wastewater treatment

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Advances in preparation,application in contaminant removal,and environmental risks of biochar-based catalysts:a review

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Biochar 2022年第1期4卷 327-357页

作者： Bowen Yang Jiawei Dai Yuan Zhao Jingwei Wu Caiya Ji Yuhu Zhang College of Resource Environment and Tourism Capital Normal UniversityBeijing 100048China School of Environmental and Safety Engineering Changzhou UniversityChangzhou 213164China

As a carbon-rich material produced by pyrolysis of biomass,biochar features low cost,large specific surface area,and widely available feedstocks based on the functional diversity and environmental-friendly properties,it has received increasing attention in the fields of Pollutant removal due to three win-win effects of water remediation,carbon sequestration and reutilization of wastes.To design excellent biochar-based catalysts for environmental applications,one must understand recent advances in the catalysts for contaminant removal.This review focuses on the current application of biochar-based catalysts in redox systems,Fenton-like systems,sonocatalytic systems and photocatalytic systems.Besides in-depth discussion in effects of preparation conditions on physicochemical characteristics of biochars,the review supplements new preparation technologies of biochar and biochar-based catalysts.Most importantly,the advantages/shortcomings,catalysis mechanisms,as well as the Pollutant removal ability of different types of biochar-based catalysts are discussed.The environmental risks of the catalyst applications are also elaborated on.Future research on biochar-based catalyst production and its environmental applications is discussed.The review provides a good overview of the current advances of biochar-based catalysts in pollutant control and the future research directions.

关键词： Biochar-based catalysts Sonocatalysts Fenton-like catalysts Photocatalysts Pollutant removal Environmental risks

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Construction of superhydrophobic directly Z-scheme bismuth oxybromide/silver phosphate fabric surface with UV shielding and enhanced visible light absorption activity

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Science China(Technological Sciences) 2021年第4期64卷 785-792页

作者： GE Bo ZHANG YuLing ZHANG TingXiao REN GuiNa LI WenZhi ZHAO Hui School of Materials Science and Engineering Liaocheng UniversityLiaocheng 252000China School of Environmental and Material Engineering Yantai UniversityYantai 264405China

Various forms of pollutants discharged from industrial and life;how to treat the opposite water-soluble pollutants at the same time is a challenge.Here,a superhydrophobic BiOBr/Ag3PO4 fabric(SH fabric)bulk material was prepared aiming at the diversity of pollutants.Water(WCA=160°)and oil contaminants(spread)have different wetting behavior on fabric surfaces.The high recovery efficiency for oil pollutants was achieved by using the selective oil removal property of the SH fabric.Meanwhile,the pollutants in the aqueous phase were removed by photocatalyst after oil/water separation.Mechanism analysis demonstrated that the direct Z-type heterojunction formed between BiOBr(EVB=1.66 eV;ECB=-1.08 eV)and Ag3PO4(EVB=3.03 eV;ECB=0.6 eV).It is worth noting that the SH fabric exhibited good mechanical stability and UV shielding performance,which have potential application in environmental control.

关键词： superhydrophobic UV shielding oil-water separation Pollutant removal

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Effects of hydraulic retention time on net present value and performance in a membrane bioreactor treating antibiotic production wastewater

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Frontiers of Environmental Science & Engineering 2020年第6期14卷 109-121页

作者： Dawei Yu Jianxing Wang Libin Zheng Qianwen Sui Hui Zhong Meixue Cheng Yuansong Wei State Key Joint Laboratory of Environmental Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Department of Water Pollution Control Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

A cost sensitivity analysis was performed for an industrial membrane bioreactor to quantify the effects of hydraulic retention times and related operational parameters on cost.Different hydraulic retention times(72-24 h)were subjected to a flat-sheet membrane bioreactor updated from an existing 72 h oxidation ditch treating antibiotic production wastewater.Field experimental data from the membrane bioreactor,both full-scale(500 m/d)and pilot(1.0 m3/d),were used to calculate the net present value(NPV),incorporating both capital expenditure(CAPEX)and operating expenditure.The results showed that the tank cost was estimated above membrane cost in the 38.2%,where capital expenditure contributed 24.2%more than operational expenditure.Tank construction cost was decisive in determining the net present value contributed 62.1%to the capital expenditure.The membrane bioreactor has the advantage of a longer lifespan flat-sheet membrane,while flux decline was tolerable.The antibiotics decreased to 1.87±0.33 mg/L in the MBR effluent.The upgrade to the membrane bioreactor also benefited further treatments by 10.1%-44.7%lower direct investment.

关键词： Antibiotic production wastewater Net present value Membrane bioreactor Hydraulic retention time Pollutant removal

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Techno-economic evaluation of a biogas-based oxidative coupling of methane process for ethylene production

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Frontiers of Chemical Science and Engineering 2018年第4期12卷 598-618页

作者： Alberto T.Penteado Mijin Kim Hamid R.Godini Erik Esche Jens-Uwe Repke Process Dynamics and Operations Group Technische Universitat BerlinD-10623 BerlinGermany

This contribution is a preliminary techno-economic assessment of a biogas-based oxidative coupling of methane (OCM) process. Biogas is frequently utilized as a renewable energy source within small scale combined heat and power plants or as a natural gas substitute. The activation of methane also enables its utilization as a feedstock to produce chemicals. In this sense, the OCM process allows for the direct conversion of methane into ethylene, which is a major building block for the chemical and polymer industries. Biogas resulting from the anaerobic digestion of vinasse, a liquid effluent from bioethanol industry, is treated for contaminant removal and its methane content is converted into ethylene, which is then purified as the main product. The biogas cleaning process is assessed based on literature data, while an experimentally validated simulation model is used to assess the OCM process. A techno-economic evaluation is then performed through a Monte Carlo simulation, wherein uncertain parameters take random values between reasonable bounds. The net present value results positive in 74% of the cases, indicating that the project is profitable under a wide range of scenarios. Some performance improvement opportunities have been identified and highlighted to guide future studies in the topic.

关键词： biogas conversion ethylene production oxidative coupling of methane feasibility study Renewable energy Monte Carlo technique Pollutant removal methane renewable energy sources Oxidative Coupling ethylene production OPERATIONAL CHANGE MEMOS chemical compounds Biogas ethylene direct conversion OCM gene

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Graphene-supported biomimetic catalysts with synergistic effect of adsorption and degradation for efficient dye capture and removal

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Chinese Chemical Letters 2020年第1期31卷 239-243页

作者： Qin Li Xiaopei Wang Xueqing Xiong Shuihong Zhu Zhaohui Meng Yongying Hong Changxu Lin Xiangyang Liu Youhui Lin Research Institute for Biomimetics and Soft Matter Department of PhysicsFujian Provincial Key Laboratory for Soft Functional Materials ResearchXiamen UniversityXiamen 361005China Department of Physics National University of SingaporeSingapore 117542Singapore

Design and development of iron porphyrin-based artificial enzymes system have been attracting a lot of attention.Herein,without any toxic reductant and harsh processing,we present a facile one-pot method to fabricate bifunctional catalytic nanocomposites consisting of graphene and hemin by using vitamin C as a mild reduction reagent.The presence of graphene helps the formation of a high degree of highly active and stable hemin on the graphene surface in a monomeric form through theirπ-πstacking interaction.As a result,such nanocomposites possess a superior adsorption capacity and intrinsic peroxidase-like catalytic activity.Moreover,by the combination of their dye adsorption ability,RGOhemin nanocomposites can serve as a suitable candidate for efficient capture and removal of dyes via a synergistic effect.Our findings may pave the way to apply graphene-supported artificial enzymes in a variety of fields,such as environmental chemistry,bionics,medicine,and biotechnology.

关键词： Nanozymes Pollutant removal Solid matrix Supported catalyst Synergistic effect

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