Switching from fossil-fuel economy to hydrogen economy requires efficient catalysts to facilitate several funda- mental electrochemical reactions,including oxygen evolution reaction (OER),hydrogen evolution reaction (...Switching from fossil-fuel economy to hydrogen economy requires efficient catalysts to facilitate several funda- mental electrochemical reactions,including oxygen evolution reaction (OER),hydrogen evolution reaction (HER),oxygen reduction reaction (ORR),and hydrogen oxidation reaction (HOR).At present,platinum-group materials are still considered as the state-of-the-art catalysts,which,however,are rare and expensive,resulting in tremendous restrictions to wide usage.The future of hydrogen economy demands the design of cost-effective and highly active catalysts that are geologically abundant, particularly for affordable and scalable device systems.As for non-platinum-group electrocatalysts,strategies to enhance their catalytic performances include controlling their size,morphology and composition,creating defects and strains,as well as modulating the van der Waals interactions and crystal phases,etc.[1,2].Although remarkable progress has been achieved,innovations in catalyst design that aim to further promote catalytic activities are still highly desired.展开更多
Efficient and stable electrocatalysts are essential for seawater splitting to sustain electrolysis without chloride corrosion,particularly at the anode.Furthermore,the oxygen evolution reaction(OER)requires high overp...Efficient and stable electrocatalysts are essential for seawater splitting to sustain electrolysis without chloride corrosion,particularly at the anode.Furthermore,the oxygen evolution reaction(OER)requires high overpotential due to the universal scaling relationship.Herein,molybdenum doping FeNi_(2)Se_(4)with lattice distortion is proposed to break the scaling relationship.Mo-FeNi_(2)Se_(4)shows high performance in direct seawater electrolysis and achieves current densities of 10 and 100 mA cm^(−2) at overpotentials of 190 and 250 mV,respectively,together with high OER selectivity and long-term stability.It is found that the lattice distortion induced by Mo doping in(3 1 0)plane of FeNi_(2)Se_(4),leads to a decrease in the d-band center and the adsorption energy of ^(*)O,which not only breaks the scaling relationship of OER but also lowers the energy barriers of rate-determining step.Moreover,it enhances the corrosion resistance to Cl^(−),and realizes the high-efficiency seawater electrolysis driven by photovoltaic.展开更多
Triboelectrification,a process that transforms mechanical energy into electrical energy through friction,holds promise for eco-friendly wastewater treatment.This study delves into the enhancement of tribocatalytic dye...Triboelectrification,a process that transforms mechanical energy into electrical energy through friction,holds promise for eco-friendly wastewater treatment.This study delves into the enhancement of tribocatalytic dye degradation using SrTiO_(3),a material notable for its non-piezoelectric and centrosymmetric properties.The synthesis of uni-and bi-doped SrTiOs particles,achieved through a solid-state reaction at 100℃,results in a high-purity cubic perovskite structure.Doping with rhodium(Rh)and carbon(C)causes crystal lattice contraction,internal stress,and significant oxygen vacancies.These changes notably improve tribocatalytic efficiency under solar irradiation,with Rh-doped SrTiO_(3) demonstrating an impressive degradation rate of approximately 88% for Rhodamine B(RhB),along with reaction rate constants near 0.9 h^(-1) at 554 nm and a noticeable blueshift.This study highlights that defects introduced by doping are integral to this process,boosting catalytic activity through energy state modification and enhancing surface redox radical production.Additionally,these defects are instrumental in generating a flexoelectric field,which markedly influences the separation of electron-hole pairs under solar irradiation.Our findings illuminate the complex interplay between material composition,defect states,and environmental conditions,paving the way for advanced strategies in environmental remediation through optimized tribocatalytic activity.展开更多
Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based...Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.展开更多
文摘Switching from fossil-fuel economy to hydrogen economy requires efficient catalysts to facilitate several funda- mental electrochemical reactions,including oxygen evolution reaction (OER),hydrogen evolution reaction (HER),oxygen reduction reaction (ORR),and hydrogen oxidation reaction (HOR).At present,platinum-group materials are still considered as the state-of-the-art catalysts,which,however,are rare and expensive,resulting in tremendous restrictions to wide usage.The future of hydrogen economy demands the design of cost-effective and highly active catalysts that are geologically abundant, particularly for affordable and scalable device systems.As for non-platinum-group electrocatalysts,strategies to enhance their catalytic performances include controlling their size,morphology and composition,creating defects and strains,as well as modulating the van der Waals interactions and crystal phases,etc.[1,2].Although remarkable progress has been achieved,innovations in catalyst design that aim to further promote catalytic activities are still highly desired.
基金financially supported by the National Natural Science Foundation of China(Nos.22471289,22478430,22101300,and 22275210)Shandong Natural Science Foundation(Nos.ZR2022ME105 and ZR2023ME004)+1 种基金Qingdao Natural Science Foundation(No.23-2-1-232-zyyd-jch)the Fundamental Research Funds for the Central Universities(Nos.22CX03010A,and 22CX01002A-1).
文摘Efficient and stable electrocatalysts are essential for seawater splitting to sustain electrolysis without chloride corrosion,particularly at the anode.Furthermore,the oxygen evolution reaction(OER)requires high overpotential due to the universal scaling relationship.Herein,molybdenum doping FeNi_(2)Se_(4)with lattice distortion is proposed to break the scaling relationship.Mo-FeNi_(2)Se_(4)shows high performance in direct seawater electrolysis and achieves current densities of 10 and 100 mA cm^(−2) at overpotentials of 190 and 250 mV,respectively,together with high OER selectivity and long-term stability.It is found that the lattice distortion induced by Mo doping in(3 1 0)plane of FeNi_(2)Se_(4),leads to a decrease in the d-band center and the adsorption energy of ^(*)O,which not only breaks the scaling relationship of OER but also lowers the energy barriers of rate-determining step.Moreover,it enhances the corrosion resistance to Cl^(−),and realizes the high-efficiency seawater electrolysis driven by photovoltaic.
基金This work was supported by the National Natural Science Foundation of China(No.11974304).
文摘Triboelectrification,a process that transforms mechanical energy into electrical energy through friction,holds promise for eco-friendly wastewater treatment.This study delves into the enhancement of tribocatalytic dye degradation using SrTiO_(3),a material notable for its non-piezoelectric and centrosymmetric properties.The synthesis of uni-and bi-doped SrTiOs particles,achieved through a solid-state reaction at 100℃,results in a high-purity cubic perovskite structure.Doping with rhodium(Rh)and carbon(C)causes crystal lattice contraction,internal stress,and significant oxygen vacancies.These changes notably improve tribocatalytic efficiency under solar irradiation,with Rh-doped SrTiO_(3) demonstrating an impressive degradation rate of approximately 88% for Rhodamine B(RhB),along with reaction rate constants near 0.9 h^(-1) at 554 nm and a noticeable blueshift.This study highlights that defects introduced by doping are integral to this process,boosting catalytic activity through energy state modification and enhancing surface redox radical production.Additionally,these defects are instrumental in generating a flexoelectric field,which markedly influences the separation of electron-hole pairs under solar irradiation.Our findings illuminate the complex interplay between material composition,defect states,and environmental conditions,paving the way for advanced strategies in environmental remediation through optimized tribocatalytic activity.
基金supported by the National Natural Science Foundation of China(22162025,22068037)the Youth Innovation Team of Shaanxi Universities+2 种基金the Open and Innovation Fund of Hubei Three Gorges Laboratory(SK232001)the Regional Innovation Capability Leading Program of Shaanxi(2022QFY07-03,2022QFY07-06)the Shaanxi Province Training Program of Innovation and Entrepreneurship for Undergraduates(S202210719108)。
文摘Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.
