Electrocatalytic CO2 reduction reaction(CO2RR)is one of the effective means to realize CO2 resource utilization.Among the high-efficiency metal-based catalysts,Cu is a star material profiting from its ability for CO2 ...Electrocatalytic CO2 reduction reaction(CO2RR)is one of the effective means to realize CO2 resource utilization.Among the high-efficiency metal-based catalysts,Cu is a star material profiting from its ability for CO2 reduction into valuable hydrocarbon products.However,due to the difficulty in activating CO2 and regulating intermediate adsorption/desorption properties,the CO2RR activity and selectivity of Cu-based catalysts still cannot meet the requirements of industrial applications.The design of Cu-based bimetallic catalysts is a potential strategy because the introduction of the second metal can well promote the activation of CO2 and break the linear scaling relationship in intermediate adsorption/desorption.In this review,the synergistic enhancements of Cu-based bimetals on CO2 activation and intermediate adsorption/desorption are analyzed in detail,including the advantages caused by the morphology of Cu-based bimetallic catalysts,the local electric field effect induced by the special nanoneedle structure,the interface engineering(strain effect,atomic arrangement,interface regulation),and other particular effects(electronic effect and tandem effect).Finally,the challenges and perspectives on the development of Cu-based bimetallic catalysts for CO2 reduction are proposed.展开更多
The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon m...The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.展开更多
The conversion of carbon dioxide(CO2)to valuable fuels and chemicals offers a new pathway for sustainable and clean carbon fixation.Recently,the focus has been on electrochemical CO2 reduction on heterogeneous electro...The conversion of carbon dioxide(CO2)to valuable fuels and chemicals offers a new pathway for sustainable and clean carbon fixation.Recently,the focus has been on electrochemical CO2 reduction on heterogeneous electrode catalysts,leading to remarkable achievements in the reaction performance.To date,CO2 to carbon monoxide(CO)conversion is considered as the most promising candidate reaction for the industrial market,owing to its high efficiency and reasonable technoeconomic feasibility.Moreover,CO has been proposed as a key intermediate species for further reduced hydrocarbons,which can pave the way for various fuel production.This study sets out to describe recent progress on the electrochemical CO2 reduction to CO in a heterogeneously catalyzed system.The review includes understanding of the catalytic material employed and engineering strategies implemented by adjusting the binding energy of key adsorbates.These material design approaches,such as nanostructuring,alloying,doping,and so forth,have pioneered breakouts in the intrinsic catalytic nature of transition metal elements.Moreover,recent advances in systematic design are summarized,with focus on practical industrial applications.Finally,perspectives on the design of electrocatalyst materials for CO production by electrochemical CO2 reduction are presented.展开更多
There have been ever-growing demands to develop advanced electrocatalysts for renewable energy conversion over the past decade.As a promising platform for advanced electrocatalysts,reduced graphene oxide(rGO)has attra...There have been ever-growing demands to develop advanced electrocatalysts for renewable energy conversion over the past decade.As a promising platform for advanced electrocatalysts,reduced graphene oxide(rGO)has attracted substantial research interests in a variety of electrochemical energy conversion reactions.Its versatile utility is mainly attributed to unique physical and chemical properties,such as high specific surface area,tunable electronic structure,and the feasibility of structural modification and functionalization.Here,a comprehensive discussion is provided upon recent advances in the material preparation,characterization,and the catalytic activity of rGO-based electrocatalysts for various electrochemical energy conversion reactions(water splitting,CO2 reduction reaction,N2 reduction reaction,and O2 reduction reaction).Major advantages of rGO and the related challenges for enhancing their catalytic performance are addressed.展开更多
The electrochemical reduction of CO2 is a promising solution for sustainable energy research and carbon emissions.However,this solution has been challenged by the lack of active and selective catalysts.Here,we report ...The electrochemical reduction of CO2 is a promising solution for sustainable energy research and carbon emissions.However,this solution has been challenged by the lack of active and selective catalysts.Here,we report a two-step synthesis of 3D ordered mesoporous Cu sphere arrays,which is fabricated by a dual template method using a poly methyl methacrylate(PMMA) inverse opal and the nonionic surfactant Brij 58 to template the mesostructure within the regular voids of a colloidal crystal.Therefo re,the well-ordered 3D interconnected bi-continuous mesopore s structure has advantages of abundant exposed catalytically active sites,efficient mass transport,and high electrical conductivity,which result in excellent electrocatalytic CO2 RR perfo rmance.The prepared 3D ordered mesoporous Cu sphere array(3 D-OMCuSA) exhibits a low onset potential of-0.4 V at a 1 mA cm^-2 electrode current density,a low Tafel slope of 109.6 mV per decade and a long-term durability in 0.1 M potassium bicarbonate.These distinct features of 3 D-OMCuSA render it a promising method for the further develo p ment of advanced electrocatalytic materials for CO2 reduction.展开更多
Electrochemical conversion of CO2 into fuels is a promising means to solve greenhouse effect and recycle chemical energy. However, the CO2 reduction reaction(CO2 RR) is limited by the high overpotential, slow kinetics...Electrochemical conversion of CO2 into fuels is a promising means to solve greenhouse effect and recycle chemical energy. However, the CO2 reduction reaction(CO2 RR) is limited by the high overpotential, slow kinetics and the accompanied side reaction of hydrogen evolution reaction. Au nanocatalysts exhibit high activity and selectivity toward the reduction of CO2 into CO. Here, we explore the Faradaic efficiency(FE)of CO2 RR catalyzed by 50 nm gold colloid and trisoctahedron. It is found that the maximum FE for CO formation on Au trisoctahedron reaches 88.80% at -0.6 V, which is 1.5 times as high as that on Au colloids(59.04% at -0.7 V). The particle-size effect of Au trisoctahedron has also been investigated, showing that the FE for CO decreases almost linearly to 62.13% when the particle diameter increases to 100 nm. The Xray diffraction characterizations together with the computational hydrogen electrode(CHE) analyses reveal that the(2 2 1) facets on Au trisoctahedron are more feasible than the(1 1 1) facets on Au colloids in stabilizing the critical intermediate COOH*, which are responsible for the higher FE and lower overpotential observed on Au trisoctahedron.展开更多
Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions a...Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright future.Especially,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) reactions.We can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction kinetics.Moreover,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction systems.Furthermore,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble process.These reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted ways.For them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of catalysts.However,the cost,synthetic methods of catalysts should also be considered.Nowadays,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so on.As extremely active fields,we should pay attention to them.Under the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.展开更多
Nanoclusters(NCs)have been demonstrated of outstanding performance in electrochemical energy storage and conversion technologies due to their strong quantum confinement effects and strong interaction with supports.Her...Nanoclusters(NCs)have been demonstrated of outstanding performance in electrochemical energy storage and conversion technologies due to their strong quantum confinement effects and strong interaction with supports.Here,we developed a class of ultrafine metal-oxide(MOx,M=Fe,Co and Ni)NCs incorporated with iron phthalocyanine(FePc),MOx/FePc-G,supported on graphene as high-performance catalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and carbon dioxide reduction(CO2RR).The high activities for ORR and OER are attributed to the electron donation and accepting ability of the highly redox active of FePc-G that could tune the properties of MOx.The FeOx/FePc-G exhibits an extremely positive half-wave potential(E1/2)of 0.888 and 0.610 V for ORR in alkaline and neutral conditions,respectively,which is around 60 mV more positive than that of Pt/C.And NiOx/FePc-G shows similar OER activity with the state-of-the-art catalysts,Ir/C,and better performance than NiFeO NCs supported on graphene.Remarkably,the CoOx/FePc-G and NiOx/FePc-G show high activity and selectivity to reduce CO2 into CO with a low onset potential of-0.22 V(overpotential is 0.11 V).展开更多
Transition metal(TM)based electrocatalysts attract increasing attention in energy conversion reactions,and current effects focus on material engineering strategies to tailor physicochemical properties of TM based elec...Transition metal(TM)based electrocatalysts attract increasing attention in energy conversion reactions,and current effects focus on material engineering strategies to tailor physicochemical properties of TM based electrocatalysts for improved performance.This review provides a summary about the recent advances of engineering TM based nanomaterials for electrocatalytic reactions,which include hydrogen evolution reaction(HER),oxygen evolution reaction(OER),CO2 reduction reaction(CO2RR),and nitrate reduction reaction(NO3RR).We highlight four engineering strategies,namely,size engineering,facet engineering,composition engineering,and crystal structure engineering for TM based electrocatalysts,and pay a special emphasis on exploring the relationship between their physicochemical properties and catalytic activities.We outline the opportunities in this research field,in particular,the strategy of rationally combining in-situ and operando techniques and theoretical predication to design efficient electrocatalysts.Finally,issues that deserve attention and consideration for practical applications are discussed.展开更多
Sn-based electrocatalysts have been gaining increasing attention due to their potential contribution in the conversion of CO2 into HCOOH driven by sustainable energy sources;however,their actual capability to catalyze...Sn-based electrocatalysts have been gaining increasing attention due to their potential contribution in the conversion of CO2 into HCOOH driven by sustainable energy sources;however,their actual capability to catalyze CO2 reduction reaction(CO2RR)still cannot meet the requirements of commercial-scale applications.Therefore developing Snbased catalyst is of vital importance.Herein,the sheet-like heterophase Sn O2/Sn3O4 with a high density of phase interfaces has been first engineered by a facile hydrothermal process,with Sn3O4 as the dominant phase.The evidences from experiments and theoretical simulation indicate that the charge redistribution and built-in electric field at heterophase interfaces boost CO2 adsorption and HCOO*formation,accelerate the charge transfer between the catalysts and reactants,and ultimately greatly elevate the intrinsic activity of the heterophase Sn O2/Sn3O4 towards CO2 RR.Meanwhile,the in-situ generated porous structure and metal Sn during CO2 RR improve the mass transmission within the interlayer volume and the conductivity of Sn O2/Sn3O4.The heterophase Sn O2/Sn3O4 displays high activity and selectivity for CO2 RR,achieving an improvement in CO2 reduction current density,88.3%Faradaic efficiency of HCOOH conversion at-0.9 VRHE,along with a long-term tolerance in CO2 RR.This study demonstrates that heterophase interface engineering is an efficient strategy to regulate advanced catalysts for different applications.展开更多
基金financial support from the International Science and Technology Cooperation Program(Grant No.2018YFE0203400 and 2017YFE0127800)the National Natural Science Foundation of China(Grant No.22002189,21872174,and U1932148)+1 种基金Hunan Provincial Natural Science Foundation(2020JJ2041,2020JJ5691)Key R&D Program of Hunan Province(2020WK2002).
文摘Electrocatalytic CO2 reduction reaction(CO2RR)is one of the effective means to realize CO2 resource utilization.Among the high-efficiency metal-based catalysts,Cu is a star material profiting from its ability for CO2 reduction into valuable hydrocarbon products.However,due to the difficulty in activating CO2 and regulating intermediate adsorption/desorption properties,the CO2RR activity and selectivity of Cu-based catalysts still cannot meet the requirements of industrial applications.The design of Cu-based bimetallic catalysts is a potential strategy because the introduction of the second metal can well promote the activation of CO2 and break the linear scaling relationship in intermediate adsorption/desorption.In this review,the synergistic enhancements of Cu-based bimetals on CO2 activation and intermediate adsorption/desorption are analyzed in detail,including the advantages caused by the morphology of Cu-based bimetallic catalysts,the local electric field effect induced by the special nanoneedle structure,the interface engineering(strain effect,atomic arrangement,interface regulation),and other particular effects(electronic effect and tandem effect).Finally,the challenges and perspectives on the development of Cu-based bimetallic catalysts for CO2 reduction are proposed.
文摘The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.
基金The authors acknowledge the support from the Korea Institute of Science and Technology(KIST)institutional program and YU-KIST convergence programpartially from National Research Foundation(NRF)funded by the Korean Government(No.2019R1A2C2005521).
文摘The conversion of carbon dioxide(CO2)to valuable fuels and chemicals offers a new pathway for sustainable and clean carbon fixation.Recently,the focus has been on electrochemical CO2 reduction on heterogeneous electrode catalysts,leading to remarkable achievements in the reaction performance.To date,CO2 to carbon monoxide(CO)conversion is considered as the most promising candidate reaction for the industrial market,owing to its high efficiency and reasonable technoeconomic feasibility.Moreover,CO has been proposed as a key intermediate species for further reduced hydrocarbons,which can pave the way for various fuel production.This study sets out to describe recent progress on the electrochemical CO2 reduction to CO in a heterogeneously catalyzed system.The review includes understanding of the catalytic material employed and engineering strategies implemented by adjusting the binding energy of key adsorbates.These material design approaches,such as nanostructuring,alloying,doping,and so forth,have pioneered breakouts in the intrinsic catalytic nature of transition metal elements.Moreover,recent advances in systematic design are summarized,with focus on practical industrial applications.Finally,perspectives on the design of electrocatalyst materials for CO production by electrochemical CO2 reduction are presented.
基金This study was supported by Korea Hydro&Nuclear Power Co.,Ltd.(No.:2018-Tech-21)the National Research Foundation of Korea(NRF)grant funded by the Korea government MSIT(2019M3E6A1064763).
文摘There have been ever-growing demands to develop advanced electrocatalysts for renewable energy conversion over the past decade.As a promising platform for advanced electrocatalysts,reduced graphene oxide(rGO)has attracted substantial research interests in a variety of electrochemical energy conversion reactions.Its versatile utility is mainly attributed to unique physical and chemical properties,such as high specific surface area,tunable electronic structure,and the feasibility of structural modification and functionalization.Here,a comprehensive discussion is provided upon recent advances in the material preparation,characterization,and the catalytic activity of rGO-based electrocatalysts for various electrochemical energy conversion reactions(water splitting,CO2 reduction reaction,N2 reduction reaction,and O2 reduction reaction).Major advantages of rGO and the related challenges for enhancing their catalytic performance are addressed.
基金This work was supported by the NSFC grant number21607113the Natural Science Foundation of Tianjin grant number 17JCQNJC07700。
文摘The electrochemical reduction of CO2 is a promising solution for sustainable energy research and carbon emissions.However,this solution has been challenged by the lack of active and selective catalysts.Here,we report a two-step synthesis of 3D ordered mesoporous Cu sphere arrays,which is fabricated by a dual template method using a poly methyl methacrylate(PMMA) inverse opal and the nonionic surfactant Brij 58 to template the mesostructure within the regular voids of a colloidal crystal.Therefo re,the well-ordered 3D interconnected bi-continuous mesopore s structure has advantages of abundant exposed catalytically active sites,efficient mass transport,and high electrical conductivity,which result in excellent electrocatalytic CO2 RR perfo rmance.The prepared 3D ordered mesoporous Cu sphere array(3 D-OMCuSA) exhibits a low onset potential of-0.4 V at a 1 mA cm^-2 electrode current density,a low Tafel slope of 109.6 mV per decade and a long-term durability in 0.1 M potassium bicarbonate.These distinct features of 3 D-OMCuSA render it a promising method for the further develo p ment of advanced electrocatalytic materials for CO2 reduction.
基金This work was supported by the National Key Research and Development Program of China(2017YFA0206500)the National Natural Science Foundation of China(21635004 and 21675079)Part of the numerical calculations were carried out in the High Performance Computing Center(HPCC)of Nanjing University.
文摘Electrochemical conversion of CO2 into fuels is a promising means to solve greenhouse effect and recycle chemical energy. However, the CO2 reduction reaction(CO2 RR) is limited by the high overpotential, slow kinetics and the accompanied side reaction of hydrogen evolution reaction. Au nanocatalysts exhibit high activity and selectivity toward the reduction of CO2 into CO. Here, we explore the Faradaic efficiency(FE)of CO2 RR catalyzed by 50 nm gold colloid and trisoctahedron. It is found that the maximum FE for CO formation on Au trisoctahedron reaches 88.80% at -0.6 V, which is 1.5 times as high as that on Au colloids(59.04% at -0.7 V). The particle-size effect of Au trisoctahedron has also been investigated, showing that the FE for CO decreases almost linearly to 62.13% when the particle diameter increases to 100 nm. The Xray diffraction characterizations together with the computational hydrogen electrode(CHE) analyses reveal that the(2 2 1) facets on Au trisoctahedron are more feasible than the(1 1 1) facets on Au colloids in stabilizing the critical intermediate COOH*, which are responsible for the higher FE and lower overpotential observed on Au trisoctahedron.
基金The financial support from the National Natural Science Foundation of China (Nos. 51772312, 21671197)
文摘Green reactions not only provide us chemical products without any pollution,but also offer us the viable technology to realize difficult tasks in normal conditions.Photo-,photoelectro-,and electrocatalytic reactions are indeed powerful tools to help us to embrace bright future.Especially,some gas-involved reactions are extremely useful to change our life environments from energy systems to liquid fuels and cost-effective products,such as H2 evolution(H2 production),02 evolution/reduction,CO2 reduction,N2 reduction(or N2 fixation) reactions.We can provide fuel cells clean H2 for electric vehicles from H2 evolution reaction(HER),at the same time,we also need highly efficient 02 reduction reaction(ORR) in fuel cells for improving the reaction kinetics.Moreover,we can get the clean oxidant O2 from water through O2 evolution reaction(OER),and carry out some reactions without posing any pollution to reaction systems.Furthermore,we can translate the greenhouse gas CO2 into useful liquid fuels through CO2 reduction reaction(CRR).Last but not the least,we can get ammonia from N2 reduction reaction(NRR),which can decrease energy input compared to the traditional Hubble process.These reactions,such as HER,ORR,OER,CRR and NRR could be realized through solar-,photoelectro-and electro-assisted ways.For them,the catalysts used play crucial roles in determining the efficiency and kinds of products,so we should consider the efficiency of catalysts.However,the cost,synthetic methods of catalysts should also be considered.Nowadays,significant progress has been achieved,however,many challenges still exist,reaction systems,catalysts underlying mechanisms,and so on.As extremely active fields,we should pay attention to them.Under the background,it has motivated us to contribute with a roadmap on ’GasInvolved Photo-and Electro-Catalysis’.
基金supported by the Australian Research Council Discovery Project Funding Scheme(project number:DP180100568)
文摘Nanoclusters(NCs)have been demonstrated of outstanding performance in electrochemical energy storage and conversion technologies due to their strong quantum confinement effects and strong interaction with supports.Here,we developed a class of ultrafine metal-oxide(MOx,M=Fe,Co and Ni)NCs incorporated with iron phthalocyanine(FePc),MOx/FePc-G,supported on graphene as high-performance catalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and carbon dioxide reduction(CO2RR).The high activities for ORR and OER are attributed to the electron donation and accepting ability of the highly redox active of FePc-G that could tune the properties of MOx.The FeOx/FePc-G exhibits an extremely positive half-wave potential(E1/2)of 0.888 and 0.610 V for ORR in alkaline and neutral conditions,respectively,which is around 60 mV more positive than that of Pt/C.And NiOx/FePc-G shows similar OER activity with the state-of-the-art catalysts,Ir/C,and better performance than NiFeO NCs supported on graphene.Remarkably,the CoOx/FePc-G and NiOx/FePc-G show high activity and selectivity to reduce CO2 into CO with a low onset potential of-0.22 V(overpotential is 0.11 V).
基金We would like to acknowledge the financial support from the National Natural Science Foundation of China(21972102)Jiangsu Highlevel Innovation and Entrepreneurial Talent Plan,the Suzhou Science and Technology Planning Project(No.SS202016)+1 种基金Natural Science Foundation for Excellent Young Scholars of Jiangsu Province(BK20180103)the Jiangsu Laboratory for Biochemical Sensing and Biochip,and Collaborative Innovation Center of Water Treatment Technology&Material.We thank Mrs Xiaoyan Wang for her help in editing the language.
文摘Transition metal(TM)based electrocatalysts attract increasing attention in energy conversion reactions,and current effects focus on material engineering strategies to tailor physicochemical properties of TM based electrocatalysts for improved performance.This review provides a summary about the recent advances of engineering TM based nanomaterials for electrocatalytic reactions,which include hydrogen evolution reaction(HER),oxygen evolution reaction(OER),CO2 reduction reaction(CO2RR),and nitrate reduction reaction(NO3RR).We highlight four engineering strategies,namely,size engineering,facet engineering,composition engineering,and crystal structure engineering for TM based electrocatalysts,and pay a special emphasis on exploring the relationship between their physicochemical properties and catalytic activities.We outline the opportunities in this research field,in particular,the strategy of rationally combining in-situ and operando techniques and theoretical predication to design efficient electrocatalysts.Finally,issues that deserve attention and consideration for practical applications are discussed.
基金the National Natural Science Foundation of China(21573062,21631004 and 21901065)the Natural Science Foundation of Heilongjiang Province(B2018008)+1 种基金the Youth Science and Technology Innovation Team Project of Heilongjiang Province(2018-KYYWF-1593)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2018009)。
文摘Sn-based electrocatalysts have been gaining increasing attention due to their potential contribution in the conversion of CO2 into HCOOH driven by sustainable energy sources;however,their actual capability to catalyze CO2 reduction reaction(CO2RR)still cannot meet the requirements of commercial-scale applications.Therefore developing Snbased catalyst is of vital importance.Herein,the sheet-like heterophase Sn O2/Sn3O4 with a high density of phase interfaces has been first engineered by a facile hydrothermal process,with Sn3O4 as the dominant phase.The evidences from experiments and theoretical simulation indicate that the charge redistribution and built-in electric field at heterophase interfaces boost CO2 adsorption and HCOO*formation,accelerate the charge transfer between the catalysts and reactants,and ultimately greatly elevate the intrinsic activity of the heterophase Sn O2/Sn3O4 towards CO2 RR.Meanwhile,the in-situ generated porous structure and metal Sn during CO2 RR improve the mass transmission within the interlayer volume and the conductivity of Sn O2/Sn3O4.The heterophase Sn O2/Sn3O4 displays high activity and selectivity for CO2 RR,achieving an improvement in CO2 reduction current density,88.3%Faradaic efficiency of HCOOH conversion at-0.9 VRHE,along with a long-term tolerance in CO2 RR.This study demonstrates that heterophase interface engineering is an efficient strategy to regulate advanced catalysts for different applications.
