Transition metals like Au,Ag,and Cu have been reported to be quite active for CO_(2) reduction.In this study,we use density functional theory(DFT)calculation to investigate the electronic structure and catalytic perfo...Transition metals like Au,Ag,and Cu have been reported to be quite active for CO_(2) reduction.In this study,we use density functional theory(DFT)calculation to investigate the electronic structure and catalytic performance of Au,Ag,Cu and their alloys for CO_(2) reduction reaction(CO_(2)RR).Theoretical calculations identified the combination of Ag,Cu,and Au in a face-centered cubic(fcc)alloy as an outstanding electrocatalyst for CO_(2) reduction to CO,with Cu as the active site.The d-orbital projected density of state(PDOS)profile suggests that alloying alters the electronic structure of the Cu site,thereby affecting the Gibbs free energy change for the formation of*COOH intermediate(ΔG_(*COOH)).To demonstrate the theoretical prediction experimentally,we employ a top-down dealloying approach to synthesize a nanoporous structured AgCuAu alloy(NP-Ag_(5)Cu_(5)Au_(5)).Electrochemical experiments validate that the ternary alloy catalyst is clearly better than unary and binary catalysts,showing a Faradaic efficiency(FE)for CO over 90%across a broad potential range of 0.6 V,with a peak of approximately 96%at-0.573 V vs.RHE.This study underscores the potential of multi-component alloys in CO_(2)RR and establishes a theoretical basis for designing efficient catalysts for CO_(2) utilization.展开更多
Aqueous zinc-ion batteries(ZIBs) are attracting considerable attention because of their low cost,high safety and abundant anode material resources.However,the major challenge faced by aqueous ZIBs is the lack of stabl...Aqueous zinc-ion batteries(ZIBs) are attracting considerable attention because of their low cost,high safety and abundant anode material resources.However,the major challenge faced by aqueous ZIBs is the lack of stable and high capacity cathode materials due to their complicated reaction mechanism and slow Zn-ion transport kinetics.This study reports a unique 3 D ’flower-like’ zinc cobaltite(ZnCo_(2)O_(4-x)) with enriched oxygen vacancies as a new cathode material for aqueous ZIBs.Computational calculations reveal that the presence of oxygen vacancies significantly enhances the electronic conductivity and accelerates Zn^(2+) diffusion by providing enlarged channels.The as-fabricated batteries present an impressive specific capacity of 148.3 mAh g^(-1) at the current density of 0.05 A g^(-1),high energy(2.8 Wh kg^(-1)) and power densities(27.2 W kg^(-1)) based on the whole device,which outperform most of the reported aqueous ZIBs.Moreover,a flexible solid-state pouch cell was demonstrated,which delivers an extremely stable capacity under bending states.This work demonstrates that the performance of Zn-ion storage can be effectively enhanced by tailoring the atomic structure of cathode materials,guiding the development of low-cost and eco-friendly energy storage materials.展开更多
The conversion of CO_(2)into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive.CuO nanosheets with an average size and thickness of~30 and~20 nm have been developed,whi...The conversion of CO_(2)into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive.CuO nanosheets with an average size and thickness of~30 and~20 nm have been developed,which are in situ reduced into Cu nanosheets during electrochemical CO_(2)reduction reaction(ECO_(2)RR).The derived Cu nanosheets demonstrate much higher selectivity for C2H4production than commercial CuO derived Cu powder,with an optimum Faradaic efficiency of 56.2%and a partial current density of C_(2)H_(4)as large as 171.0 mA cm^(-2)in a gas diffusion flow cell.The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5(4–6),which facilitates the formation of^(*)CHO rather than^(*)COH intermediate,meanwhile boosting the C-C coupling reaction of^(*)CO and^(*)CHO intermediates,which are the critical steps for C_(2)H_(4)formation.展开更多
Background:Structural birth defects occur in approximately 3%of live births;most such defects lack defined genetic or environmental causes.Despite advances in surgical approaches,pharmacologic prevention remains large...Background:Structural birth defects occur in approximately 3%of live births;most such defects lack defined genetic or environmental causes.Despite advances in surgical approaches,pharmacologic prevention remains largely out of reach.Methods:We queried worldwide databases of 20,248 families that included children with neurodevelopmental disorders and that were enriched for parental consanguinity.Approximately one third of affected children in these families presented with structural birth defects or microcephaly.展开更多
基金supported by Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application(No.ZDSYS20220527171407017)。
文摘Transition metals like Au,Ag,and Cu have been reported to be quite active for CO_(2) reduction.In this study,we use density functional theory(DFT)calculation to investigate the electronic structure and catalytic performance of Au,Ag,Cu and their alloys for CO_(2) reduction reaction(CO_(2)RR).Theoretical calculations identified the combination of Ag,Cu,and Au in a face-centered cubic(fcc)alloy as an outstanding electrocatalyst for CO_(2) reduction to CO,with Cu as the active site.The d-orbital projected density of state(PDOS)profile suggests that alloying alters the electronic structure of the Cu site,thereby affecting the Gibbs free energy change for the formation of*COOH intermediate(ΔG_(*COOH)).To demonstrate the theoretical prediction experimentally,we employ a top-down dealloying approach to synthesize a nanoporous structured AgCuAu alloy(NP-Ag_(5)Cu_(5)Au_(5)).Electrochemical experiments validate that the ternary alloy catalyst is clearly better than unary and binary catalysts,showing a Faradaic efficiency(FE)for CO over 90%across a broad potential range of 0.6 V,with a peak of approximately 96%at-0.573 V vs.RHE.This study underscores the potential of multi-component alloys in CO_(2)RR and establishes a theoretical basis for designing efficient catalysts for CO_(2) utilization.
基金supported by the National Natural Science Foundation of China(Nos.51873198,51503184 and 21703248)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB20000000)+1 种基金the Engineering and Physical Sciences Research Council(EPSRC,EP/R023581/1)the RSC Mobility Grant(M19-7656)and the STFC Batteries Network(ST/R006873/1)。
文摘Aqueous zinc-ion batteries(ZIBs) are attracting considerable attention because of their low cost,high safety and abundant anode material resources.However,the major challenge faced by aqueous ZIBs is the lack of stable and high capacity cathode materials due to their complicated reaction mechanism and slow Zn-ion transport kinetics.This study reports a unique 3 D ’flower-like’ zinc cobaltite(ZnCo_(2)O_(4-x)) with enriched oxygen vacancies as a new cathode material for aqueous ZIBs.Computational calculations reveal that the presence of oxygen vacancies significantly enhances the electronic conductivity and accelerates Zn^(2+) diffusion by providing enlarged channels.The as-fabricated batteries present an impressive specific capacity of 148.3 mAh g^(-1) at the current density of 0.05 A g^(-1),high energy(2.8 Wh kg^(-1)) and power densities(27.2 W kg^(-1)) based on the whole device,which outperform most of the reported aqueous ZIBs.Moreover,a flexible solid-state pouch cell was demonstrated,which delivers an extremely stable capacity under bending states.This work demonstrates that the performance of Zn-ion storage can be effectively enhanced by tailoring the atomic structure of cathode materials,guiding the development of low-cost and eco-friendly energy storage materials.
基金funded by the National Key Research and Development Program of China(2017YFA0700103,2018YFA0704502)the National Natural Science Foundation of China(21703248)staffs in BL11B beamline in Shanghai Synchrotron Radiation Facility(SSRF)for their technical assistance(2020-SSRF-PT-012223 and 2021-SSRF-PT-015319)。
文摘The conversion of CO_(2)into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive.CuO nanosheets with an average size and thickness of~30 and~20 nm have been developed,which are in situ reduced into Cu nanosheets during electrochemical CO_(2)reduction reaction(ECO_(2)RR).The derived Cu nanosheets demonstrate much higher selectivity for C2H4production than commercial CuO derived Cu powder,with an optimum Faradaic efficiency of 56.2%and a partial current density of C_(2)H_(4)as large as 171.0 mA cm^(-2)in a gas diffusion flow cell.The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5(4–6),which facilitates the formation of^(*)CHO rather than^(*)COH intermediate,meanwhile boosting the C-C coupling reaction of^(*)CO and^(*)CHO intermediates,which are the critical steps for C_(2)H_(4)formation.
文摘Background:Structural birth defects occur in approximately 3%of live births;most such defects lack defined genetic or environmental causes.Despite advances in surgical approaches,pharmacologic prevention remains largely out of reach.Methods:We queried worldwide databases of 20,248 families that included children with neurodevelopmental disorders and that were enriched for parental consanguinity.Approximately one third of affected children in these families presented with structural birth defects or microcephaly.
