Catalytic converting CO2 into fuels with the help of solar energy is regarded as‘dream reaction’,as both energy crisis and environmental issue can be mitigated simultaneously.However,it is still suffering from low e...Catalytic converting CO2 into fuels with the help of solar energy is regarded as‘dream reaction’,as both energy crisis and environmental issue can be mitigated simultaneously.However,it is still suffering from low efficiency due to narrow solar-spectrum utilization and sluggish heterogeneous reaction kinetics.In this work,we demonstrate that catalytic reduction of CO2 can be achieved over Au nanoparticles(NPs)deposited rutile under full solar-spectrum irradiation,boosted by solar-heating effect.We found that UV and visible light can initiate the reaction,and the heat from IR light and local surface-plasmon resonance relaxation of Au NPs can boost the reaction kinetically.The apparent activation energy is determined experimentally and is used to explain the superior catalytic activity of Au/rutile to rutile in a kinetic way.We also find the photo-thermal synergy in the Au/rutile system.We envision that this work may facilitate understanding the kinetics of CO2 reduction and developing feasible catalytic systems with full solar spectrum utilization for practical artificial photosynthesis.展开更多
The transformation of CO_(2)into cyclic carbonates via atom-economical cycloadditions with epoxides has recently attracted tremendous attention.On one hand,though many heterogeneous catalysts have been developed for t...The transformation of CO_(2)into cyclic carbonates via atom-economical cycloadditions with epoxides has recently attracted tremendous attention.On one hand,though many heterogeneous catalysts have been developed for this reaction,they typically suffer from disadvantages such as the need for severe reaction conditions,catalyst loss,and large amounts of soluble co-catalysts.On the other hand,the development of heterogeneous catalysts featuring multiple and cooperative active sites,remains challenging and desirable.In this study,we prepared a series of porous organic catalysts(POP-PBnCl-TPPMg-x)via the copolymerization metal-porphyrin compounds and phosphonium salt monomers in various ratios.The resulting materials contain both Lewis-acidic and Lewis-basic active sites.The molecular-level combination of these sites in the same polymer allows these active sites to work synergistically,giving rise to excellent performance in the cycloaddition reaction of CO_(2)with epoxides,under mild conditions(40℃ and 1 atm CO_(2))in the absence of soluble co-catalysts.POP-PBnCl-TPPMg-12 can also efficiently fixate CO_(2)under low-CO_(2)-concentration(15%v/v N2)conditions representative of typical CO_(2)compositions in industrial exhaust gases.More importantly,this catalyst shows excellent recyclability and can easily be separated and reused at least five times while maintaining its activity.In view of their heterogeneous nature and excellent catalytic performance,the obtained catalysts are promising candidates for the transformation of industrially generated CO_(2)into high value-added chemicals.展开更多
Sustainable conversion of carbon dioxide(CO_(2))to high value-added chemicals and fuels is a promising solution to solve the problem of excessive CO_(2) emissions and alleviate the shortage of fossil fuels,maintaining...Sustainable conversion of carbon dioxide(CO_(2))to high value-added chemicals and fuels is a promising solution to solve the problem of excessive CO_(2) emissions and alleviate the shortage of fossil fuels,maintaining the balance of the carbon cycle in nature.The development of catalytic system is of great significance to improve the efficiency and selectivity for electrochemical CO_(2) conversion.In particular,bismuth(Bi)based catalysts are the most promising candidates,while confronting challenges.This review aims to elucidate the fundamental issues of efficient and stable Bi-based catalysts,constructing a bridge between the category,synthesis approach and electrochemical performance.In this review,the categories of Bi-based catalysts are firstly introduced,such as metals,alloys,single atoms,compounds and composites.Followed by the statement of the reliable and versatile synthetic approaches,the representative optimization strategies,such as morphology manipulation,defect engineering,component and heterostructure regulation,have been highlighted in the discussion,paving in-depth insight upon the design principles,reaction activity,selectivity and stability.Afterward,in situ characterization techniques will be discussed to illustrate the mechanisms of electrochemical CO_(2) conversion.In the end,the challenges and perspectives are also provided,promoting a systematic understanding in terms of the bottleneck and opportunities in the field of electrochemical CO_(2) conversion.展开更多
Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing issue.As a clean and efficient energy conversion process,electrocatalytic r...Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing issue.As a clean and efficient energy conversion process,electrocatalytic reduction can reduce carbon dioxide into a series of alcohols and acidic organic molecules,which can effectively realize the utilization and transformation of carbon dioxide.This review focuses on the tuning strategies and structure effects of catalysts for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).The tuning strategies for the active sites of catalysts have been reviewed from intrinsic and external perspectives.The structure effects for the CO_(2)RR catalysts have also been discussed,such as tandem catalysis,synergistic effects and confinement catalysis.We expect that this review about tuning strategies and structure effects can provide guidance for designing highly efficient CO_(2)RR electrocatalysts.展开更多
基金supported by the Belt and Road Initiative by Chinese Academy of Sciencesthe National Natural Science Foundation of China(21673052,11404074)
文摘Catalytic converting CO2 into fuels with the help of solar energy is regarded as‘dream reaction’,as both energy crisis and environmental issue can be mitigated simultaneously.However,it is still suffering from low efficiency due to narrow solar-spectrum utilization and sluggish heterogeneous reaction kinetics.In this work,we demonstrate that catalytic reduction of CO2 can be achieved over Au nanoparticles(NPs)deposited rutile under full solar-spectrum irradiation,boosted by solar-heating effect.We found that UV and visible light can initiate the reaction,and the heat from IR light and local surface-plasmon resonance relaxation of Au NPs can boost the reaction kinetically.The apparent activation energy is determined experimentally and is used to explain the superior catalytic activity of Au/rutile to rutile in a kinetic way.We also find the photo-thermal synergy in the Au/rutile system.We envision that this work may facilitate understanding the kinetics of CO2 reduction and developing feasible catalytic systems with full solar spectrum utilization for practical artificial photosynthesis.
文摘The transformation of CO_(2)into cyclic carbonates via atom-economical cycloadditions with epoxides has recently attracted tremendous attention.On one hand,though many heterogeneous catalysts have been developed for this reaction,they typically suffer from disadvantages such as the need for severe reaction conditions,catalyst loss,and large amounts of soluble co-catalysts.On the other hand,the development of heterogeneous catalysts featuring multiple and cooperative active sites,remains challenging and desirable.In this study,we prepared a series of porous organic catalysts(POP-PBnCl-TPPMg-x)via the copolymerization metal-porphyrin compounds and phosphonium salt monomers in various ratios.The resulting materials contain both Lewis-acidic and Lewis-basic active sites.The molecular-level combination of these sites in the same polymer allows these active sites to work synergistically,giving rise to excellent performance in the cycloaddition reaction of CO_(2)with epoxides,under mild conditions(40℃ and 1 atm CO_(2))in the absence of soluble co-catalysts.POP-PBnCl-TPPMg-12 can also efficiently fixate CO_(2)under low-CO_(2)-concentration(15%v/v N2)conditions representative of typical CO_(2)compositions in industrial exhaust gases.More importantly,this catalyst shows excellent recyclability and can easily be separated and reused at least five times while maintaining its activity.In view of their heterogeneous nature and excellent catalytic performance,the obtained catalysts are promising candidates for the transformation of industrially generated CO_(2)into high value-added chemicals.
文摘Sustainable conversion of carbon dioxide(CO_(2))to high value-added chemicals and fuels is a promising solution to solve the problem of excessive CO_(2) emissions and alleviate the shortage of fossil fuels,maintaining the balance of the carbon cycle in nature.The development of catalytic system is of great significance to improve the efficiency and selectivity for electrochemical CO_(2) conversion.In particular,bismuth(Bi)based catalysts are the most promising candidates,while confronting challenges.This review aims to elucidate the fundamental issues of efficient and stable Bi-based catalysts,constructing a bridge between the category,synthesis approach and electrochemical performance.In this review,the categories of Bi-based catalysts are firstly introduced,such as metals,alloys,single atoms,compounds and composites.Followed by the statement of the reliable and versatile synthetic approaches,the representative optimization strategies,such as morphology manipulation,defect engineering,component and heterostructure regulation,have been highlighted in the discussion,paving in-depth insight upon the design principles,reaction activity,selectivity and stability.Afterward,in situ characterization techniques will be discussed to illustrate the mechanisms of electrochemical CO_(2) conversion.In the end,the challenges and perspectives are also provided,promoting a systematic understanding in terms of the bottleneck and opportunities in the field of electrochemical CO_(2) conversion.
文摘Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing issue.As a clean and efficient energy conversion process,electrocatalytic reduction can reduce carbon dioxide into a series of alcohols and acidic organic molecules,which can effectively realize the utilization and transformation of carbon dioxide.This review focuses on the tuning strategies and structure effects of catalysts for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).The tuning strategies for the active sites of catalysts have been reviewed from intrinsic and external perspectives.The structure effects for the CO_(2)RR catalysts have also been discussed,such as tandem catalysis,synergistic effects and confinement catalysis.We expect that this review about tuning strategies and structure effects can provide guidance for designing highly efficient CO_(2)RR electrocatalysts.
