Electrochemical CO_(2)reduction reaction(CO_(2)RR)into high-value chemicals and fuels is recognized as a promising strategy for mitigating energy and environmental challenges.However,this process frequently faces limi...Electrochemical CO_(2)reduction reaction(CO_(2)RR)into high-value chemicals and fuels is recognized as a promising strategy for mitigating energy and environmental challenges.However,this process frequently faces limitations due to inadequate selectivity towards specific products and insufficient electrochemical stability.Main group indium(In)catalysts have emerged as promising materials for CO_(2)RR to highly valued formate.In this study,we constructed an indium cluster material with charge-asymmetric atomic structure anchored on nitrogen-free carbon nanoframeworks(designated as In Clu/C),which exhibits exceptional efficiency as a CO_(2)RR catalyst for formate production.Notably,the In Clu/C achieves a remarkable formate Faradaic efficiency of 98.7%at−0.70 V.Furthermore,in-situ X-ray absorption spectroscopy(XAS)measurements reveal that the superior catalytic performance can be attributed to partially positively charged In^(δ+)(0<δ<3)active sites.This discovery may provide new insights into the precise synthesis of metal cluster catalysts for environmental and energy applications.展开更多
Transition metal sulfides with homogeneous multi-metallic elements promise high catalytic performance for water electrolysis owing to the unique structure and highly tailorable electrochemical property.Most existing s...Transition metal sulfides with homogeneous multi-metallic elements promise high catalytic performance for water electrolysis owing to the unique structure and highly tailorable electrochemical property.Most existing synthetic routes require high temperature to ensure the uniform mixing of various elements,making the synthesis highly challenging.Here,for the first-time novel carbon fiber supported high-entropy Co-Zn-Cd-Cu-Mn sulfide(CoZnCdCuMnS@CF)nanoarrays are fabricated by the mild cation exchange strategy.Benefiting from the synergistic effect among multiple metals and the strong interfacial bonding between high-entropy Co-Zn-Cd-Cu-Mn sulfide nanoarrays and the carbon fiber support,CoZnCdCuMnS@CF exhibits superior catalytic activity and stability toward overall water splitting in alkaline medium.Impressively,CoZnCdCuMnS@CF only needs low overpotentials of 173 and 220 mV to reach the current density of 10 mA•cm^(−2),with excellent durability for over 70 and 113 h for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)respectively.More importantly,the bifunctional electrode(CoZnCdCuMnS@CF||CoZnCdCuMnS@CF)for overall water splitting can deliver a small cell voltage of 1.63 V to afford 10 mA•cm^(−2) and exhibit outstanding stability of negligible decay after 73 h continuous operation.This work provides a viable synthesis route toward advanced high-entropy materials with great potential applications.展开更多
Rational design and construction of low-cost and highly efficient electrocatalysts for hydrogen evolution reaction(HER)is meaningful but challenging.Herein,a robust three dimensional(3D)hollow CoSe_(2)@ultrathin MoSe_...Rational design and construction of low-cost and highly efficient electrocatalysts for hydrogen evolution reaction(HER)is meaningful but challenging.Herein,a robust three dimensional(3D)hollow CoSe_(2)@ultrathin MoSe_(2)core@shell heterostructure(CoSe_(2)@MoSe_(2))is proposed as an efficient HER electrocatalyst through interfacial engineering.Benefitting from the abundant heterogeneous interfaces on CoSe_(2)@MoSe_(2),the exposed edge active sites are maximized and the charge transfer at the hetero-interfaces is accelerated,thus facilitating the HER kinetics.It exhibits remarkable performance in pH-universal conditions.Notably,it only needs an overpotential(η10)of 108 mV to reach a current density of 10 mA·cm^(-2)in 1.0 M KOH,outperforming most of the reported transition metal selenides electrocatalysts.Density functional theory(DFT)calculations unveil that the heterointerfaces synergistically optimize the Gibbs free energies of H2O and H^(*)during alkaline HER,accelerating the reaction kinetics.The present work may provide new construction guidance for rational design of high-efficient electrocatalysts.展开更多
基金supported by the National Natural Science Foundation of China(No.22201262)Natural Science Foundation of Henan(No.252300421175)+1 种基金the University Natural Science Research Project of Anhui Province(No.2024AH040186)the Application Project of Bengbu Univerisity(No.2024YYX28QD).
文摘Electrochemical CO_(2)reduction reaction(CO_(2)RR)into high-value chemicals and fuels is recognized as a promising strategy for mitigating energy and environmental challenges.However,this process frequently faces limitations due to inadequate selectivity towards specific products and insufficient electrochemical stability.Main group indium(In)catalysts have emerged as promising materials for CO_(2)RR to highly valued formate.In this study,we constructed an indium cluster material with charge-asymmetric atomic structure anchored on nitrogen-free carbon nanoframeworks(designated as In Clu/C),which exhibits exceptional efficiency as a CO_(2)RR catalyst for formate production.Notably,the In Clu/C achieves a remarkable formate Faradaic efficiency of 98.7%at−0.70 V.Furthermore,in-situ X-ray absorption spectroscopy(XAS)measurements reveal that the superior catalytic performance can be attributed to partially positively charged In^(δ+)(0<δ<3)active sites.This discovery may provide new insights into the precise synthesis of metal cluster catalysts for environmental and energy applications.
基金The authors thank the National Natural Science Foundation of China(No.U1804140)China Postdoctoral Science Foundation(No.2021M702939)for support.
文摘Transition metal sulfides with homogeneous multi-metallic elements promise high catalytic performance for water electrolysis owing to the unique structure and highly tailorable electrochemical property.Most existing synthetic routes require high temperature to ensure the uniform mixing of various elements,making the synthesis highly challenging.Here,for the first-time novel carbon fiber supported high-entropy Co-Zn-Cd-Cu-Mn sulfide(CoZnCdCuMnS@CF)nanoarrays are fabricated by the mild cation exchange strategy.Benefiting from the synergistic effect among multiple metals and the strong interfacial bonding between high-entropy Co-Zn-Cd-Cu-Mn sulfide nanoarrays and the carbon fiber support,CoZnCdCuMnS@CF exhibits superior catalytic activity and stability toward overall water splitting in alkaline medium.Impressively,CoZnCdCuMnS@CF only needs low overpotentials of 173 and 220 mV to reach the current density of 10 mA•cm^(−2),with excellent durability for over 70 and 113 h for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)respectively.More importantly,the bifunctional electrode(CoZnCdCuMnS@CF||CoZnCdCuMnS@CF)for overall water splitting can deliver a small cell voltage of 1.63 V to afford 10 mA•cm^(−2) and exhibit outstanding stability of negligible decay after 73 h continuous operation.This work provides a viable synthesis route toward advanced high-entropy materials with great potential applications.
基金The authors thank the National Natural Science Foundation of China(Nos.U1804140,U20041100 and 21801015)for supportThis work is also supported by Beijing Institute of Technology Research Fund Program for Young Scholars(No.3090012221909).
文摘Rational design and construction of low-cost and highly efficient electrocatalysts for hydrogen evolution reaction(HER)is meaningful but challenging.Herein,a robust three dimensional(3D)hollow CoSe_(2)@ultrathin MoSe_(2)core@shell heterostructure(CoSe_(2)@MoSe_(2))is proposed as an efficient HER electrocatalyst through interfacial engineering.Benefitting from the abundant heterogeneous interfaces on CoSe_(2)@MoSe_(2),the exposed edge active sites are maximized and the charge transfer at the hetero-interfaces is accelerated,thus facilitating the HER kinetics.It exhibits remarkable performance in pH-universal conditions.Notably,it only needs an overpotential(η10)of 108 mV to reach a current density of 10 mA·cm^(-2)in 1.0 M KOH,outperforming most of the reported transition metal selenides electrocatalysts.Density functional theory(DFT)calculations unveil that the heterointerfaces synergistically optimize the Gibbs free energies of H2O and H^(*)during alkaline HER,accelerating the reaction kinetics.The present work may provide new construction guidance for rational design of high-efficient electrocatalysts.
