Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radica...Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radical-based iron(Fe^(2+)),both used for the degradation of bisphenol A(BPA).The N-CNTs/PDS system,driven by the electron transfer mechanism,achieved remarkable 90.9%BPA removal within 30 min at high BPA concentrations,significantly outperforming the Fe^(2+)/PDS system,which attained only 38.9%removal.The N-CNTs/PDS system maintained robust degradation efficiency across a wide range of BPA concentrations and exhibited a high degree of resilience in diverse water matrices.By directly abstracting electrons from BPA molecules,the N-CNTs/PDS system effectively minimised oxidant wastage and mitigated the risk of secondary pollution,ensuring efficient utilisation of active sites on N-CNTs and sustaining a high catalytic rate.The formation of the N-CNTs-PDS^(*)complex significantly enhanced BPA degradation and mineralisation,thereby optimising PDS consumption.These findings highlight the unparalleled advantages of the N-CNTs/PDS system in managing complex wastewater,offering a promising and innovative solution for treating complex industrial wastewater and advancing environmental remediation efforts.展开更多
The degradation capacity of advanced oxidants generated from oxygen reduction was investigated in model effluent containing chlorobenzene, aniline and benzene through the advanced oxidation processes(AOPs). Intermedia...The degradation capacity of advanced oxidants generated from oxygen reduction was investigated in model effluent containing chlorobenzene, aniline and benzene through the advanced oxidation processes(AOPs). Intermediate products of the degradation process were determined by GC–MS, and they contributed to specify the degradation pathways of monoaromatic compounds. The study particularly focused on the influence of the dosage of the oxidant, pH and the initial concentration of organic compounds on the degradation effectiveness.When the dosage of oxidant was 4 wt% and the pH was 7, the maximum degradation rates of 74.83% chlorobenzene, 70.32% aniline and 37.69% benzene were achieved. Furthermore, microwave was applied to intensify the oxidation process under optimal operation conditions, and the degradation rates were increased to 87.85% chlorobenzene, 89.11% aniline and 39.03% benzene, respectively.展开更多
As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing ant...As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing antibiotics from wastewater, H_(2)O_(2)-based advanced oxidation processes(AOPs) have received increasing attention due to their fast reaction rate and strong oxidation capability. Hence this review critically discusses:(i) Recent research progress of AOPs with the addition of H_(2)O_(2) for antibiotics removal through different methods of H_(2)O_(2) activation;(ii) recent advances in AOPs that can in-situ generate and activate H_(2)O_(2) for antibiotics removal;(iii) H_(2)O_(2)-based AOPs as a combination with other techniques for the degradation and mineralization of antibiotics in wastewater. Future perspectives about H_(2)O_(2)-based AOPs are also presented to grasp the future research trend in the area.展开更多
The degradation of metoprolol(MTP)by the UV/sulfite with oxygen as an advanced reduction process(ARP)and that without oxygen as an advanced oxidation process(AOP)was comparatively studied herein.The degradation of MTP...The degradation of metoprolol(MTP)by the UV/sulfite with oxygen as an advanced reduction process(ARP)and that without oxygen as an advanced oxidation process(AOP)was comparatively studied herein.The degradation of MTP by both processes followed the first-order rate law with comparable reaction rate constants of 1.50×10^(-3)sec^(−1)and 1.20×10^(-3)sec^(−1),respectively.Scavenging experiments demonstrated that both e^(−)_(aq)and H·played a crucial role in MTP degradation by the UV/sulfite as an ARP,while SO_(4)^(·−)was the dominant oxidant in the UV/sulfite AOP.The degradation kinetics of MTP by the UV/sulfite as an ARP and AOP shared a similar pH dependence with a minimum rate obtained around pH 8.The results could be well explained by the pH impacts on the MTP speciation and sulfite species.Totally six transformation products(TPs)were identified from MTP degradation by the UV/sulfite ARP,and two additional ones were detected in the UV/sulfite AOP.The benzene ring and ether groups of MTP were proposed as the major reactive sites for both processes based on molecular orbital calculations by density functional theory(DFT).The similar degradation products of MTP by the UV/sulfite process as an ARP and AOP indicated that e^(−)_(aq)/H·and SO_(4)^(·−)might share similar reaction mechanisms,primarily including hydroxylation,dealkylation,and H abstraction.The toxicity of MTP solution treated by the UV/sulfite AOP was calculated to be higher than that in the ARP by the Ecological Struc-ture Activity Relationships(ECOSAR)software,due to the accumulation of TPs with higher toxicity.展开更多
A modified advanced oxidation process(AOP) utilizing a UV/electrochemically-generated peroxide system was used to fabricate titania films on chemically polished NiTi shape memory alloy(SMA). The microstructure and bio...A modified advanced oxidation process(AOP) utilizing a UV/electrochemically-generated peroxide system was used to fabricate titania films on chemically polished NiTi shape memory alloy(SMA). The microstructure and biomedical properties of the film were characterized by scanning electron microscopy(SEM), X-ray photoelectron spectroscopy(XPS), inductively-coupled plasma mass spectrometry(ICPMS), hemolysis analysis, and blood platelet adhesion test. It is found that the modified AOP has a high processing effectiveness and can result in the formation of a dense titania film with a Ni-free zone near its top surface. In comparison, Ni can still be detected on the outer NiTi surface by the conventional AOP using the UV/H2O2 system. The depth profiles of O, Ni, Ti show that the film possesses a smooth graded interface structure next to the NiTi substrate and this structure enhances the mechanical stability of titania film. The titania film can dramatically reduce toxic Ni ion release and also improve the hemolysis resistance and thromboresistance of biomedical NiTi SMA.展开更多
Advanced oxidation processes(AOPs)governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation.Nevertheless,the low diffusion rates,inadequate...Advanced oxidation processes(AOPs)governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation.Nevertheless,the low diffusion rates,inadequate interactions of the reactants,and limited active site exposure hinder treatment efficiency.Porous carbocatalysts with high specific surface area,tunable pore size,and programmable active sites demonstrate outstanding performance in activating diverse types of peroxides to generate active species for treatment of aqueous organic pollutants.The pore-rich structures enhance reaction kinetics for peroxide activation by facilitating diffusion of the reactants and their interactions.Additionally,the structural flexibility of porous structures favors the accommodation of highly dispersed metal species and allows for precise tuning of the microenvironment around the active sites,which further enhances the catalytic activity.This review critically summarizes the recent research progress in the applications of engineered porous carbocatalysts for peroxide activation and outlines the prevailing pore construction methods in carbocatalysts.Moreover,engineering strategies to regulate the mass transfer efficiency and fine-tune the microenvironment around the active sites are systematically addressed to enhance their catalytic peroxide activation performances.Challenges and future research opportunities pertaining to the design,optimization,mechanistic investigation,and practical application of porous carbocatalysts in peroxide activation are also proposed.展开更多
Brominated flame retardants(BFRs),have been extensively utilized in modern industry,contaminate aquatic ecosystems.They exhibit bioaccumulation and biomagnification properties,posing significant risks to human health,...Brominated flame retardants(BFRs),have been extensively utilized in modern industry,contaminate aquatic ecosystems.They exhibit bioaccumulation and biomagnification properties,posing significant risks to human health,such as developmental disorders,endocrine disruption,and other adverse effects.Current treatment methods for BFRs encompass chemical,electrochemical,biological,and advanced oxidation processes(AOPs).Among them,AOPs are particularly notable for their stability,ease of control,and production of clean end-products.This paper focuses on employing a titanium dioxide(TiO_(2))photocatalytic system to investigate the degradation of 2,4,6-tribromophenol(TBP).展开更多
Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality...Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality,hidden contamination,and complex treatment requirements.Current research focuses on advanced treatment technologies,among which the advanced oxidation process(AOPs) of peroxomonosulfate(PMS) has great potential.Although there are many reviews of PMS-based AOP,most of them focus on surface water.This review aims to explore the activation reaction of PMS to groundwater by in-situ chemical oxidation(ISCO) technology,further study the reaction mechanism,compare the treatment effect of characteristic pollutants in the groundwater of the chemical industry park,propose new activation methods and catalyst selection,and provide guidance for future groundwater treatment research.展开更多
A method for oxidative degradation of 1,4-dioxane （1,4-D） in waste water using a combination of ozone oxidation with UV irradiation （ozone/UV） treatment was investigated. The results showed that 1,4-D was degraded...A method for oxidative degradation of 1,4-dioxane （1,4-D） in waste water using a combination of ozone oxidation with UV irradiation （ozone/UV） treatment was investigated. The results showed that 1,4-D was degraded by ozone/UV treatment up to 90 min. The optimum concentration for the injected ozone gas was about 40 g·m^3 under a constant level of UV irradiation. Furthermore, solid phase extraction and GC-MS analysis showed no specific or reproducible peaks due to by-products of 1,4-D. It was therefore concluded that 1,4-D was completely degraded by ozone/UV treatment. In contrast, the amount of 1,4-D remaining decreased slowly in the presence of HCOf or CI. It was suggested that the degradation of 1,4-D, which results from .OH oxidation, was retarded by the presence of HCO3 or CI, which act as radical scavengers.展开更多
With the escalating global challenges of energy scarcity and environmental pollution,the development of efficient and sustainable catalytic technologies has become imperative.Dual-atom catalysts(DACs)have garnered con...With the escalating global challenges of energy scarcity and environmental pollution,the development of efficient and sustainable catalytic technologies has become imperative.Dual-atom catalysts(DACs)have garnered considerable interest,particularly in various catalytic processes,demonstrating exceptional promise in enhancing reaction efficiency and selectivity.Unlike prior reviews that primarily emphasized a specific or single reaction process,this review provides a systematic and comprehensive analysis of DACs across diverse oxidation chemistry,including ozone oxidation,Fenton-like reactions,photo/electro/piezo-catalysis,and enzyme-mimetic oxidation.It begins with a concise overview of the discovery,development,and evolution of DACs,together with an in-depth investigation of diverse synthesis strategies and state-of-the-art characterization techniques.Moreover,the remarkable improvement in the performance of DACs in catalytic processes is discussed on the basis of how their geometric microstructure and electronic configuration,including charge transfer,coordination environment,and spin state,influence catalytic kinetics and thermodynamics,exploring the relationships between the structural geometry,electronic interactions,and catalysis mechanisms of DACs.By integrating these multidimensional insights,this review expands conventional paradigms in the development of DACs and identifies innovative pathways for linking their microstructure and catalysis mechanism.Finally,we emphasize critical research gaps and emerging opportunities for DACs that warrant further exploration and attention.This review would provide valuable guidance and foundation in the rapidly evolving field of DACs.展开更多
针对当前鞍钢鲅鱼圈焦化废水处理系统水质不稳的相关问题,在原有“A 2+O+混凝沉淀”和“臭氧催化氧化+B A F”工艺基础上,新增“A O P高级氧化”单元和“超滤+反渗透”膜单元,提升了出水水质。引入中水回用技术后废水回用率达到70%以上...针对当前鞍钢鲅鱼圈焦化废水处理系统水质不稳的相关问题,在原有“A 2+O+混凝沉淀”和“臭氧催化氧化+B A F”工艺基础上,新增“A O P高级氧化”单元和“超滤+反渗透”膜单元,提升了出水水质。引入中水回用技术后废水回用率达到70%以上,解决了焦化废水平衡问题。展开更多
基金supported by the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2024LHMS05048).
文摘Addressing the growing challenge of water contamination,this study comparatively evaluated a persulfate(PDS)system activated by nonradical nitrogen-doped carbon nanotubes(N-CNTs)versus a PDS system activated by radical-based iron(Fe^(2+)),both used for the degradation of bisphenol A(BPA).The N-CNTs/PDS system,driven by the electron transfer mechanism,achieved remarkable 90.9%BPA removal within 30 min at high BPA concentrations,significantly outperforming the Fe^(2+)/PDS system,which attained only 38.9%removal.The N-CNTs/PDS system maintained robust degradation efficiency across a wide range of BPA concentrations and exhibited a high degree of resilience in diverse water matrices.By directly abstracting electrons from BPA molecules,the N-CNTs/PDS system effectively minimised oxidant wastage and mitigated the risk of secondary pollution,ensuring efficient utilisation of active sites on N-CNTs and sustaining a high catalytic rate.The formation of the N-CNTs-PDS^(*)complex significantly enhanced BPA degradation and mineralisation,thereby optimising PDS consumption.These findings highlight the unparalleled advantages of the N-CNTs/PDS system in managing complex wastewater,offering a promising and innovative solution for treating complex industrial wastewater and advancing environmental remediation efforts.
基金Supported by the Key Technologies R&D Program of China(2011BAE111300)
文摘The degradation capacity of advanced oxidants generated from oxygen reduction was investigated in model effluent containing chlorobenzene, aniline and benzene through the advanced oxidation processes(AOPs). Intermediate products of the degradation process were determined by GC–MS, and they contributed to specify the degradation pathways of monoaromatic compounds. The study particularly focused on the influence of the dosage of the oxidant, pH and the initial concentration of organic compounds on the degradation effectiveness.When the dosage of oxidant was 4 wt% and the pH was 7, the maximum degradation rates of 74.83% chlorobenzene, 70.32% aniline and 37.69% benzene were achieved. Furthermore, microwave was applied to intensify the oxidation process under optimal operation conditions, and the degradation rates were increased to 87.85% chlorobenzene, 89.11% aniline and 39.03% benzene, respectively.
基金financially supported by National Natural Science Foundation of China(Nos.21976096,52170085 and 21773129)Tianjin Development Program for Innovation and Entrepreneurship+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(No.2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University。
文摘As important emerging contaminants, antibiotics have caused potential hazards to the ecological environment and human health due to their extensive production and consumption. Among various techniques for removing antibiotics from wastewater, H_(2)O_(2)-based advanced oxidation processes(AOPs) have received increasing attention due to their fast reaction rate and strong oxidation capability. Hence this review critically discusses:(i) Recent research progress of AOPs with the addition of H_(2)O_(2) for antibiotics removal through different methods of H_(2)O_(2) activation;(ii) recent advances in AOPs that can in-situ generate and activate H_(2)O_(2) for antibiotics removal;(iii) H_(2)O_(2)-based AOPs as a combination with other techniques for the degradation and mineralization of antibiotics in wastewater. Future perspectives about H_(2)O_(2)-based AOPs are also presented to grasp the future research trend in the area.
基金This study was supported by the Guangdong introducing innovative and entrepreneurial teams(No.2019ZT08L213)the Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(No.GML2019ZD0403)+2 种基金the National Natural Science Foundation of China(Nos.51979044 and 42177045)the Young Talent Project of Beijing Normal University at Zhuhai(No.310432101)We also thank the support received from China Scholarship Council(CSC)for providing a graduate fellowship to Y.C.(No.202006120356).
文摘The degradation of metoprolol(MTP)by the UV/sulfite with oxygen as an advanced reduction process(ARP)and that without oxygen as an advanced oxidation process(AOP)was comparatively studied herein.The degradation of MTP by both processes followed the first-order rate law with comparable reaction rate constants of 1.50×10^(-3)sec^(−1)and 1.20×10^(-3)sec^(−1),respectively.Scavenging experiments demonstrated that both e^(−)_(aq)and H·played a crucial role in MTP degradation by the UV/sulfite as an ARP,while SO_(4)^(·−)was the dominant oxidant in the UV/sulfite AOP.The degradation kinetics of MTP by the UV/sulfite as an ARP and AOP shared a similar pH dependence with a minimum rate obtained around pH 8.The results could be well explained by the pH impacts on the MTP speciation and sulfite species.Totally six transformation products(TPs)were identified from MTP degradation by the UV/sulfite ARP,and two additional ones were detected in the UV/sulfite AOP.The benzene ring and ether groups of MTP were proposed as the major reactive sites for both processes based on molecular orbital calculations by density functional theory(DFT).The similar degradation products of MTP by the UV/sulfite process as an ARP and AOP indicated that e^(−)_(aq)/H·and SO_(4)^(·−)might share similar reaction mechanisms,primarily including hydroxylation,dealkylation,and H abstraction.The toxicity of MTP solution treated by the UV/sulfite AOP was calculated to be higher than that in the ARP by the Ecological Struc-ture Activity Relationships(ECOSAR)software,due to the accumulation of TPs with higher toxicity.
基金Project(NCET-06-0464) supported by the Program for New Century Excellent Talents in University of Ministry of Education of ChinaProject(BK2007515) supported by the Natural Science Foundation of Jiangsu Province, China+2 种基金Project(2006AA03Z445) supported by the National High-tech Research and Development Program of ChinaProject supported by Nippon Sheet Glass Foundation for Materials Science and Engineering (NSG Foundation)Project(7001999) supported by SRG Grant from the Research Committee of the CityU of HK
文摘A modified advanced oxidation process(AOP) utilizing a UV/electrochemically-generated peroxide system was used to fabricate titania films on chemically polished NiTi shape memory alloy(SMA). The microstructure and biomedical properties of the film were characterized by scanning electron microscopy(SEM), X-ray photoelectron spectroscopy(XPS), inductively-coupled plasma mass spectrometry(ICPMS), hemolysis analysis, and blood platelet adhesion test. It is found that the modified AOP has a high processing effectiveness and can result in the formation of a dense titania film with a Ni-free zone near its top surface. In comparison, Ni can still be detected on the outer NiTi surface by the conventional AOP using the UV/H2O2 system. The depth profiles of O, Ni, Ti show that the film possesses a smooth graded interface structure next to the NiTi substrate and this structure enhances the mechanical stability of titania film. The titania film can dramatically reduce toxic Ni ion release and also improve the hemolysis resistance and thromboresistance of biomedical NiTi SMA.
基金supports from the National Natural Science Foundation of China(Nos.22478426 and 22278436)Young Elite Scientists Sponsorship Program by BAST(No.1101020370359)Science Foundation of China University of Petroleum,Beijing(No.2462021QNXZ009)。
文摘Advanced oxidation processes(AOPs)governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation.Nevertheless,the low diffusion rates,inadequate interactions of the reactants,and limited active site exposure hinder treatment efficiency.Porous carbocatalysts with high specific surface area,tunable pore size,and programmable active sites demonstrate outstanding performance in activating diverse types of peroxides to generate active species for treatment of aqueous organic pollutants.The pore-rich structures enhance reaction kinetics for peroxide activation by facilitating diffusion of the reactants and their interactions.Additionally,the structural flexibility of porous structures favors the accommodation of highly dispersed metal species and allows for precise tuning of the microenvironment around the active sites,which further enhances the catalytic activity.This review critically summarizes the recent research progress in the applications of engineered porous carbocatalysts for peroxide activation and outlines the prevailing pore construction methods in carbocatalysts.Moreover,engineering strategies to regulate the mass transfer efficiency and fine-tune the microenvironment around the active sites are systematically addressed to enhance their catalytic peroxide activation performances.Challenges and future research opportunities pertaining to the design,optimization,mechanistic investigation,and practical application of porous carbocatalysts in peroxide activation are also proposed.
文摘Brominated flame retardants(BFRs),have been extensively utilized in modern industry,contaminate aquatic ecosystems.They exhibit bioaccumulation and biomagnification properties,posing significant risks to human health,such as developmental disorders,endocrine disruption,and other adverse effects.Current treatment methods for BFRs encompass chemical,electrochemical,biological,and advanced oxidation processes(AOPs).Among them,AOPs are particularly notable for their stability,ease of control,and production of clean end-products.This paper focuses on employing a titanium dioxide(TiO_(2))photocatalytic system to investigate the degradation of 2,4,6-tribromophenol(TBP).
基金supported by the National Key Research and Development Program of China (No.2023YFC3708005)the National Natural Science Foundation of China (Nos.21872102,22172080)the Fundamental Research Funds for the Central Universities (Nankai University,No.63241208)。
文摘Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality,hidden contamination,and complex treatment requirements.Current research focuses on advanced treatment technologies,among which the advanced oxidation process(AOPs) of peroxomonosulfate(PMS) has great potential.Although there are many reviews of PMS-based AOP,most of them focus on surface water.This review aims to explore the activation reaction of PMS to groundwater by in-situ chemical oxidation(ISCO) technology,further study the reaction mechanism,compare the treatment effect of characteristic pollutants in the groundwater of the chemical industry park,propose new activation methods and catalyst selection,and provide guidance for future groundwater treatment research.
文摘A method for oxidative degradation of 1,4-dioxane （1,4-D） in waste water using a combination of ozone oxidation with UV irradiation （ozone/UV） treatment was investigated. The results showed that 1,4-D was degraded by ozone/UV treatment up to 90 min. The optimum concentration for the injected ozone gas was about 40 g·m^3 under a constant level of UV irradiation. Furthermore, solid phase extraction and GC-MS analysis showed no specific or reproducible peaks due to by-products of 1,4-D. It was therefore concluded that 1,4-D was completely degraded by ozone/UV treatment. In contrast, the amount of 1,4-D remaining decreased slowly in the presence of HCOf or CI. It was suggested that the degradation of 1,4-D, which results from .OH oxidation, was retarded by the presence of HCO3 or CI, which act as radical scavengers.
基金supported by the National Natural Science Foundation of China(52300045)the China Postdoctoral Science Foundation(2023M741424)+1 种基金the Jiangsu Province Natural Science Fund(BK20241025)the Start-up Fund for Introduced Scholar of Jiangsu University(5501370025).
文摘With the escalating global challenges of energy scarcity and environmental pollution,the development of efficient and sustainable catalytic technologies has become imperative.Dual-atom catalysts(DACs)have garnered considerable interest,particularly in various catalytic processes,demonstrating exceptional promise in enhancing reaction efficiency and selectivity.Unlike prior reviews that primarily emphasized a specific or single reaction process,this review provides a systematic and comprehensive analysis of DACs across diverse oxidation chemistry,including ozone oxidation,Fenton-like reactions,photo/electro/piezo-catalysis,and enzyme-mimetic oxidation.It begins with a concise overview of the discovery,development,and evolution of DACs,together with an in-depth investigation of diverse synthesis strategies and state-of-the-art characterization techniques.Moreover,the remarkable improvement in the performance of DACs in catalytic processes is discussed on the basis of how their geometric microstructure and electronic configuration,including charge transfer,coordination environment,and spin state,influence catalytic kinetics and thermodynamics,exploring the relationships between the structural geometry,electronic interactions,and catalysis mechanisms of DACs.By integrating these multidimensional insights,this review expands conventional paradigms in the development of DACs and identifies innovative pathways for linking their microstructure and catalysis mechanism.Finally,we emphasize critical research gaps and emerging opportunities for DACs that warrant further exploration and attention.This review would provide valuable guidance and foundation in the rapidly evolving field of DACs.
