We studied the decomposition of two haloacetic acids (HAAs),dichloroacetic acid (DCAA) and trichloroacetic acid (TCAA),in water by single oxidants ozone (O3) and ultraviolet radiation (UV) and the advanced oxidation p...We studied the decomposition of two haloacetic acids (HAAs),dichloroacetic acid (DCAA) and trichloroacetic acid (TCAA),in water by single oxidants ozone (O3) and ultraviolet radiation (UV) and the advanced oxidation processes (AOPs) constituted by the combinations of O3/UV,H2O2/UV,O3 /H2O2,and O3/H2O2/UV. The concentrations of HAAs were analyzed at specified time intervals to track their decomposition. Except for O3 and UV,the four combined oxidation processes remarkably enhance the decomposition of DCAA and TCAA owing to the generated very reactive hydroxyl radicals. The fastest decomposition process is O3/H2O2/UV,closely followed by O3/UV. DCAA is much easier to decompose than TCAA. The kinetics of HAA decomposition by O3/UV can be described well by a pseudo first-order reaction model under a constant initial dissolved O3 concentration and fixed UV radiation. Humic acids and HCO3-in the reaction system both decrease the decomposition rate constants for DCAA and TCAA. The amount of H2O2 accumulates in the presence of humic acids in the O3/UV process.展开更多
Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illust...Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.展开更多
Human society is currently facing significant and pressing issues in the form of serious environmental pollution and energy shortages,which have arisen owing to the rapid development of the economy and contemporary in...Human society is currently facing significant and pressing issues in the form of serious environmental pollution and energy shortages,which have arisen owing to the rapid development of the economy and contemporary industry.Photocatalysis has considerable potential as a viable technique for providing sustainable and environmentally friendly energy sources.The use of lanthanide-based photocatalysts on supporting substrates has garnered significant attention over the past decade within the scope of organic pollution remediation.Owing to its unique and promising bandgap,electrical conductivity,and stability,traditional GdVO_(4)exhibits remarkable photocatalytic performance with ongoing advances and advancements.This review provides an overview of the latest advancements in the modification techniques employed for GdVO_(4)-based photocatalysts,with a specific focus on their application in the photocatalytic degradation of organic pollutants.The supplied information provides a concise overview of current obstacles,limitations,advancements,mechanisms,and potential prospects for new opportunities.This review is anticipated to provide a significant reference and scientific justification for the active development of GdVO_(4)-based materials for environmental applications.展开更多
TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its el...TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its electrochemical activity.Herein,narrow bandgap manganese oxide(MnO_(x))was composited with TiO_(2)nanotube arrays(TiO_(2)NTAs)that in-situ oxidized on porous Ti sponge,forming the MnO_(x)-TiO_(2)NTAs anode.XANES and XPS analysis further proved that the composition of MnO_(x)is Mn2O3.Electrochemical characterizations revealed that increasing the composited concentration of MnO_(x)can improve the conductivity and reduce oxygen evolution potential so as to improve the electrochemical activity of the composited MnO_(x)-TiO_(2)NTAs anode.Meanwhile,the optimal degradation rate of benzoic acid(BA)was achieved using MnO_(x)-TiO_(2)NTAs with a MnO_(x)concentration of 0.1 mmol L^(-1),and the role of MnO_(x)was proposed based on DFT calculation.Additionally,the required electrical energy(EE/O)to destroy BA was optimized by varying the composited concentration of MnO_(x)and the degradation voltage.These quantitative results are of great significance for the design and application of high-performance materials for EAOPs.展开更多
Non-thermal plasma has emerged as an effective treatment system against the latest class of highly recalcitrant and toxic environmental pollutants termed emerging contaminants(ECs).In the present work,a detailed exper...Non-thermal plasma has emerged as an effective treatment system against the latest class of highly recalcitrant and toxic environmental pollutants termed emerging contaminants(ECs).In the present work,a detailed experimental study is carried out to evaluate the efficacy of a non-thermal plasma jet with two dyes,Rd.B and Met.Blue,as model contaminants.The plasma jet provided a complete dye decoloration in 30 min with an applied voltage of 6.5 kV_(p-p).·OH,having the highest oxidation potential,acts as the main reactive species,which with direct action on contaminants also acts indirectly by getting converted into H_(2)O_(2)and O_(3).Further,the effect of critical operational parameters viz,sample pH,applied voltage(4.5–6.5 kV_(p-p)),conductivity(5–20 mS cm^(-1)),and sample distance on plasma treatment efficacy was also examined.Out of all the assessed parameters,the applied voltage and sample conductivity was found to be the most significant operating parameters.A high voltage and low conductivity favored the dye decoloration,while the pH effect was not that significant.To understand the influence of plasma discharge gas on treatment efficacy,all the experiments are conducted with argon and helium gases under the fixed geometrical configuration.Both the gases provided a similar dye decoloration efficiency.The DBD plasma system with complete dye removal also rendered maximum mineralization of 73%for Rd.B,and 60%for Met.Blue.Finally,the system's efficiency against the actual ECs(four pharmaceutical compounds,viz,metformin,atenolol,acetaminophen,and ranitidine)and microbial contaminant(E.coli)was also tested.The system showed effectivity in the complete removal of targeted pharmaceuticals and a log2.5 E.coli reduction.The present systematic characterization of dye degradation could be of interest to large communities working towards commercializing plasma treatment systems.展开更多
In the electrical discharge plasma process, various chemical and physical processes can participate in the removal of contaminants. In this paper, the chemical and physical processes that occur as a result of the elec...In the electrical discharge plasma process, various chemical and physical processes can participate in the removal of contaminants. In this paper, the chemical and physical processes that occur as a result of the electrical discharge plasma are reviewed, and their possible roles in the degradation of contaminants are discussed. Measurement methods for the quantification of important reactive species and their advantages and shortcomings are presented. Approaches on how to enhance the diffusion of the reactive species in solution are examined. In addition, the formation of typical reactive species in different electrical discharge plasma is compared.展开更多
Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and stor...Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and storage,value-added chemical synthesis and environmental remediation.However,their environmental appli-cations lack of a comprehensive summary and in-depth discussion.In this review,recent progresses in synthesis routes and advanced characterization techniques for 2D SACs are introduced,and a comprehensive discussion on their applications in environmental remediation is presented.Generally,2D SACs can be effective in catalytic elimination of aqueous and gaseous pollutants via radical or non-radical routes and transformation of toxic pollutants into less poisonous species or highly value-added products,opening a new horizon for the contami-nant treatment.In addition,in-depth reaction mechanisms and potential pathways are systematically discussed,and the relationship between the structure-performance is highlighted.Finally,several critical challenges within this field are presented,and possible directions for further explorations of 2D SACs in environmental remediation are suggested.Although the research of 2D SACs in the environmental application is still in its infancy,this review will provide a timely summary on the emerging field,and would stimulate tremendous interest for designing more attractive 2D SACs and promoting their wide applications.展开更多
基金Natural Science Foundation of Chongqing under Grant No. CSTC2008BB7299.
文摘We studied the decomposition of two haloacetic acids (HAAs),dichloroacetic acid (DCAA) and trichloroacetic acid (TCAA),in water by single oxidants ozone (O3) and ultraviolet radiation (UV) and the advanced oxidation processes (AOPs) constituted by the combinations of O3/UV,H2O2/UV,O3 /H2O2,and O3/H2O2/UV. The concentrations of HAAs were analyzed at specified time intervals to track their decomposition. Except for O3 and UV,the four combined oxidation processes remarkably enhance the decomposition of DCAA and TCAA owing to the generated very reactive hydroxyl radicals. The fastest decomposition process is O3/H2O2/UV,closely followed by O3/UV. DCAA is much easier to decompose than TCAA. The kinetics of HAA decomposition by O3/UV can be described well by a pseudo first-order reaction model under a constant initial dissolved O3 concentration and fixed UV radiation. Humic acids and HCO3-in the reaction system both decrease the decomposition rate constants for DCAA and TCAA. The amount of H2O2 accumulates in the presence of humic acids in the O3/UV process.
基金financially supported by National Key R&D Program International Cooperation Project(2023YFE0108100)Natural Science Foundation of China(No.52170085)+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.
文摘Human society is currently facing significant and pressing issues in the form of serious environmental pollution and energy shortages,which have arisen owing to the rapid development of the economy and contemporary industry.Photocatalysis has considerable potential as a viable technique for providing sustainable and environmentally friendly energy sources.The use of lanthanide-based photocatalysts on supporting substrates has garnered significant attention over the past decade within the scope of organic pollution remediation.Owing to its unique and promising bandgap,electrical conductivity,and stability,traditional GdVO_(4)exhibits remarkable photocatalytic performance with ongoing advances and advancements.This review provides an overview of the latest advancements in the modification techniques employed for GdVO_(4)-based photocatalysts,with a specific focus on their application in the photocatalytic degradation of organic pollutants.The supplied information provides a concise overview of current obstacles,limitations,advancements,mechanisms,and potential prospects for new opportunities.This review is anticipated to provide a significant reference and scientific justification for the active development of GdVO_(4)-based materials for environmental applications.
基金the support from the Brook Byers Institute for Sustainable Systems,Hightower ChairGeorgia Research Alliance at the Georgia Institute of Technology。
文摘TiO_(2)has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs)due to its structural stability and high oxygen overpotential.However,there is still much room for improving its electrochemical activity.Herein,narrow bandgap manganese oxide(MnO_(x))was composited with TiO_(2)nanotube arrays(TiO_(2)NTAs)that in-situ oxidized on porous Ti sponge,forming the MnO_(x)-TiO_(2)NTAs anode.XANES and XPS analysis further proved that the composition of MnO_(x)is Mn2O3.Electrochemical characterizations revealed that increasing the composited concentration of MnO_(x)can improve the conductivity and reduce oxygen evolution potential so as to improve the electrochemical activity of the composited MnO_(x)-TiO_(2)NTAs anode.Meanwhile,the optimal degradation rate of benzoic acid(BA)was achieved using MnO_(x)-TiO_(2)NTAs with a MnO_(x)concentration of 0.1 mmol L^(-1),and the role of MnO_(x)was proposed based on DFT calculation.Additionally,the required electrical energy(EE/O)to destroy BA was optimized by varying the composited concentration of MnO_(x)and the degradation voltage.These quantitative results are of great significance for the design and application of high-performance materials for EAOPs.
基金supported by grants from the IIT Delhi FIRP program grant (No. MI02081)
文摘Non-thermal plasma has emerged as an effective treatment system against the latest class of highly recalcitrant and toxic environmental pollutants termed emerging contaminants(ECs).In the present work,a detailed experimental study is carried out to evaluate the efficacy of a non-thermal plasma jet with two dyes,Rd.B and Met.Blue,as model contaminants.The plasma jet provided a complete dye decoloration in 30 min with an applied voltage of 6.5 kV_(p-p).·OH,having the highest oxidation potential,acts as the main reactive species,which with direct action on contaminants also acts indirectly by getting converted into H_(2)O_(2)and O_(3).Further,the effect of critical operational parameters viz,sample pH,applied voltage(4.5–6.5 kV_(p-p)),conductivity(5–20 mS cm^(-1)),and sample distance on plasma treatment efficacy was also examined.Out of all the assessed parameters,the applied voltage and sample conductivity was found to be the most significant operating parameters.A high voltage and low conductivity favored the dye decoloration,while the pH effect was not that significant.To understand the influence of plasma discharge gas on treatment efficacy,all the experiments are conducted with argon and helium gases under the fixed geometrical configuration.Both the gases provided a similar dye decoloration efficiency.The DBD plasma system with complete dye removal also rendered maximum mineralization of 73%for Rd.B,and 60%for Met.Blue.Finally,the system's efficiency against the actual ECs(four pharmaceutical compounds,viz,metformin,atenolol,acetaminophen,and ranitidine)and microbial contaminant(E.coli)was also tested.The system showed effectivity in the complete removal of targeted pharmaceuticals and a log2.5 E.coli reduction.The present systematic characterization of dye degradation could be of interest to large communities working towards commercializing plasma treatment systems.
基金funded by National Natural Science Foundation of China (Nos. 51608448 and 21737003)Young Talent Cultivation Scheme Funding of Northwest A&F University (No. Z109021802)the Fundamental Research Funds for the Central Universities (No. Z109021617) for their financial support in this research
文摘In the electrical discharge plasma process, various chemical and physical processes can participate in the removal of contaminants. In this paper, the chemical and physical processes that occur as a result of the electrical discharge plasma are reviewed, and their possible roles in the degradation of contaminants are discussed. Measurement methods for the quantification of important reactive species and their advantages and shortcomings are presented. Approaches on how to enhance the diffusion of the reactive species in solution are examined. In addition, the formation of typical reactive species in different electrical discharge plasma is compared.
基金This work was financially supported by the National Natural Science Foundation of China(51602133,51876093)China MOST(2018YFE0183600).
文摘Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and storage,value-added chemical synthesis and environmental remediation.However,their environmental appli-cations lack of a comprehensive summary and in-depth discussion.In this review,recent progresses in synthesis routes and advanced characterization techniques for 2D SACs are introduced,and a comprehensive discussion on their applications in environmental remediation is presented.Generally,2D SACs can be effective in catalytic elimination of aqueous and gaseous pollutants via radical or non-radical routes and transformation of toxic pollutants into less poisonous species or highly value-added products,opening a new horizon for the contami-nant treatment.In addition,in-depth reaction mechanisms and potential pathways are systematically discussed,and the relationship between the structure-performance is highlighted.Finally,several critical challenges within this field are presented,and possible directions for further explorations of 2D SACs in environmental remediation are suggested.Although the research of 2D SACs in the environmental application is still in its infancy,this review will provide a timely summary on the emerging field,and would stimulate tremendous interest for designing more attractive 2D SACs and promoting their wide applications.
