High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailo...High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailorable electronic structure,and entropy stabilization effect.The precise fabrication of HEMs with functional nanostructures provides a crucial avenue to optimize the adsorption strength and catalytic activity for electrocatalysis.This review comprehensively summarizes the development of HEMs,focusing on the principles and strategies of structural design,and the catalytic mechanism towards hydrogen evolution reaction,oxygen evolution reaction and oxygen reduction reaction for the development of high-performance electrocatalysts.The complexity inherent in the interactions between different elements,the changes in the d-band center and the Gibbs free energies during the catalytic progress,as well as the coordination environment of the active sites associated with the unique crystal structure to improve the catalytic performance are discussed.We also provide a perspective on the challenges and future development direction of HEMs in electrocatalysis.This review will contribute to the design and development of HEMs-based catalysts for the next generation of electrochemical applications.展开更多
This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degra...This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.展开更多
Molybdenum-based materials have been intensively investigated for high-performance gas sensor applications.Particularly,molybdenum oxides and dichalcogenides nanostructures have been widely examined due to their tunab...Molybdenum-based materials have been intensively investigated for high-performance gas sensor applications.Particularly,molybdenum oxides and dichalcogenides nanostructures have been widely examined due to their tunable structural and physicochemical properties that meet sensor requirements.These materials have good durability,are naturally abundant,low cost,and have facile preparation,allowing scalable fabrication to fulfill the growing demand of susceptible sensor devices.Significant advances have been made in recent decades to design and fabricate various molybdenum oxides-and dichalcogenides-based sensing materials,though it is still challenging to achieve high performances.Therefore,many experimental and theoretical investigations have been devoted to exploring suitable approaches which can significantly enhance their gas sensing properties.This review comprehensively examines recent advanced strategies to improve the nanostructured molybdenum-based material performance for detecting harmful pollutants,dangerous gases,or even exhaled breath monitoring.The summary and future challenges to advance their gas sensing performances will also be presented.展开更多
Rare earth elements (REEs), comprising 17 % of known elements, are pivotal in diverse industries. Despitetheir name, they are not geologically rare but dispersed, posing challenges for economically viablemining. This ...Rare earth elements (REEs), comprising 17 % of known elements, are pivotal in diverse industries. Despitetheir name, they are not geologically rare but dispersed, posing challenges for economically viablemining. This review explores the environmental and health implications of REEs, emphasizing theiremerging status as contaminants in aquatic environments, raising health concerns through the foodchain. The necessity to recover REEs from wastewater demands efficient methods, particularly focusingon adsorption. Spinel ferrites (SFs), characterized by superparamagnetism and thermal stability, aregaining prominence in this context. Utilizing metal cations like Fe, Co, Ni, Mn, Zn, and Cu, SF-basedmagnetic nanocomposites exhibit remarkable efficiency in adsorbing REEs. This article delves intoadsorption mechanisms, including electrostatic interactions and ion exchange, highlighting the advantagesof stability, biocompatibility, and cost-effectiveness associated with SFs. SF-based nanocomposites,offering scalability and effectiveness at low concentrations, emerge as a promising solution foraddressing environmental concerns related to REEs while meeting the escalating demand for theseessential elements.展开更多
We study the carbon dioxide reduction reaction(CO_(2)RR)activity and selectivity of Fe single-atom catalyst(Fe-SAC)and Fe dual-atom catalyst(Fe-DAC)active sites at the interior of graphene and the edges of graphitic n...We study the carbon dioxide reduction reaction(CO_(2)RR)activity and selectivity of Fe single-atom catalyst(Fe-SAC)and Fe dual-atom catalyst(Fe-DAC)active sites at the interior of graphene and the edges of graphitic nanopore by using a combination of DFT calculations and microkinetic simulations.The trend of limiting potentials for CO_(2)RR to produce CO can be described by using either the adsorption energy of COOH,CO,or their combination.CO_(2)RR process with reasonable reaction rates can be achieved only on the active site configurations with weak tendencies toward CO poisoning.The efficiency of CO_(2)RR on a catalyst depends on its ability to suppress the parasitic hydrogen evolution reaction(HER),which is directly related to the behavior of H adsorption on the catalyst’s active site.We find that the edges of the graphitic nanopore can act as potential adsorption sites for an H atom,and in some cases,the edge site can bind the H atom much stronger than the main Fe site.The linear scaling between CO and H adsorptions is broken if this condition is met.This condition also allows some edge active site configurations to have their CO_(2)RR limiting potential lower than the HER process favoring CO production over H2 production.展开更多
基金supported by the Guangdong Basic and Applied Basic Research Fund Project(2022A1515140061,No.11000-2344014)Startup Foundation for Postdoctor by Dongguan University of Technology(No.11000-221110149)the High-level Talents Program(contract number 2023JC10L014)of the Department of Science and Technology of Guangdong Province。
文摘High entropy materials(HEMs)are the promising electrocatalysts for anion exchange membrane electrolyser(AEMs)and proton exchange membrane fuel cells(PEMFCs)due to the intriguing cocktail effect,wide design space,tailorable electronic structure,and entropy stabilization effect.The precise fabrication of HEMs with functional nanostructures provides a crucial avenue to optimize the adsorption strength and catalytic activity for electrocatalysis.This review comprehensively summarizes the development of HEMs,focusing on the principles and strategies of structural design,and the catalytic mechanism towards hydrogen evolution reaction,oxygen evolution reaction and oxygen reduction reaction for the development of high-performance electrocatalysts.The complexity inherent in the interactions between different elements,the changes in the d-band center and the Gibbs free energies during the catalytic progress,as well as the coordination environment of the active sites associated with the unique crystal structure to improve the catalytic performance are discussed.We also provide a perspective on the challenges and future development direction of HEMs in electrocatalysis.This review will contribute to the design and development of HEMs-based catalysts for the next generation of electrochemical applications.
基金supported by the Financial Supports of the National Natural Science Foundation of China(Nos.51508056,52370030 and 42007352)the Chongqing Postgraduate Joint Training Base Project(No.JDLHPYJD2022005)the special fund of Henan Key Labora-tory of Water Pollution Control and Rehabilitation Technology(No.CJSZ2024001).
文摘This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.
基金partly supported by the JSPS Grant-in-Aid for Scientific Research(No.JP16H06439,No.20H00297)by the Dynamic Alliance for Open Innovation Bridging Human,Environment and Materials in Network Joint Research Center for Materialsfinancial grants provided by Indonesia Ministry of Education,Culture,Research,and Technology,under the scheme of Basic Research Program No.2/E1/KP.PTNBH/2021 managed by Institut Teknologi Bandung。
文摘Molybdenum-based materials have been intensively investigated for high-performance gas sensor applications.Particularly,molybdenum oxides and dichalcogenides nanostructures have been widely examined due to their tunable structural and physicochemical properties that meet sensor requirements.These materials have good durability,are naturally abundant,low cost,and have facile preparation,allowing scalable fabrication to fulfill the growing demand of susceptible sensor devices.Significant advances have been made in recent decades to design and fabricate various molybdenum oxides-and dichalcogenides-based sensing materials,though it is still challenging to achieve high performances.Therefore,many experimental and theoretical investigations have been devoted to exploring suitable approaches which can significantly enhance their gas sensing properties.This review comprehensively examines recent advanced strategies to improve the nanostructured molybdenum-based material performance for detecting harmful pollutants,dangerous gases,or even exhaled breath monitoring.The summary and future challenges to advance their gas sensing performances will also be presented.
文摘Rare earth elements (REEs), comprising 17 % of known elements, are pivotal in diverse industries. Despitetheir name, they are not geologically rare but dispersed, posing challenges for economically viablemining. This review explores the environmental and health implications of REEs, emphasizing theiremerging status as contaminants in aquatic environments, raising health concerns through the foodchain. The necessity to recover REEs from wastewater demands efficient methods, particularly focusingon adsorption. Spinel ferrites (SFs), characterized by superparamagnetism and thermal stability, aregaining prominence in this context. Utilizing metal cations like Fe, Co, Ni, Mn, Zn, and Cu, SF-basedmagnetic nanocomposites exhibit remarkable efficiency in adsorbing REEs. This article delves intoadsorption mechanisms, including electrostatic interactions and ion exchange, highlighting the advantagesof stability, biocompatibility, and cost-effectiveness associated with SFs. SF-based nanocomposites,offering scalability and effectiveness at low concentrations, emerge as a promising solution foraddressing environmental concerns related to REEs while meeting the escalating demand for theseessential elements.
基金supported by the Ministry of Education,Culture,Research,and Technology of the Republic of Indonesia through the‘WCR 2022’program under contract number 007/E5/PG.02.00.PT/2022.
文摘We study the carbon dioxide reduction reaction(CO_(2)RR)activity and selectivity of Fe single-atom catalyst(Fe-SAC)and Fe dual-atom catalyst(Fe-DAC)active sites at the interior of graphene and the edges of graphitic nanopore by using a combination of DFT calculations and microkinetic simulations.The trend of limiting potentials for CO_(2)RR to produce CO can be described by using either the adsorption energy of COOH,CO,or their combination.CO_(2)RR process with reasonable reaction rates can be achieved only on the active site configurations with weak tendencies toward CO poisoning.The efficiency of CO_(2)RR on a catalyst depends on its ability to suppress the parasitic hydrogen evolution reaction(HER),which is directly related to the behavior of H adsorption on the catalyst’s active site.We find that the edges of the graphitic nanopore can act as potential adsorption sites for an H atom,and in some cases,the edge site can bind the H atom much stronger than the main Fe site.The linear scaling between CO and H adsorptions is broken if this condition is met.This condition also allows some edge active site configurations to have their CO_(2)RR limiting potential lower than the HER process favoring CO production over H2 production.
