Ammonia plays an essential role in human production and life as a raw material for chemical fertilizers.The nitrate electroreduction to ammonia reaction(NO_(3)RR)has garnered attention due to its advantages over the H...Ammonia plays an essential role in human production and life as a raw material for chemical fertilizers.The nitrate electroreduction to ammonia reaction(NO_(3)RR)has garnered attention due to its advantages over the Haber-Bosch process and electrochemical nitrogen reduction reaction.Therefore,it represents a promising approach to safeguard the ecological environment by enabling the cycling of nitrogen species.This review begins by discussing the theoretical insights of the NO_(3)RR.It then summarizes recent advances in catalyst design and construction strategies,including alloying,structure engineering,surface engineering,and heterostructure engineering.Finally,the challenges and prospects in this field are presented.This review aims to guide for enhancing the efficiency of electrocatalysts in the NO_(3)RR,and offers insights for converting NO_(3)-to NH_(3).展开更多
Selective semihydrogenation of acetylene in raw olefin streams to ethylene is a key industrial reaction to produce polymer-grade feeds for the manufacture of corresponding polymers.The currently used process in indust...Selective semihydrogenation of acetylene in raw olefin streams to ethylene is a key industrial reaction to produce polymer-grade feeds for the manufacture of corresponding polymers.The currently used process in industry is the thermocatalytic acetylene semihydrogenation with pressurized hydrogen and Pd-based catalysts at relatively high temperatures.The high cost of Pd urgently desires the design of non-noble metal-based catalysts.However,non-noble metal-based catalysts commonly require much higher reaction temperatures than Pd-based catalysts because of their poor intrinsic activity.Therefore,aiming at increasing economic efficiency and sustainability,various strategies are explored for developing non-noble metal-based catalysts for thermocatalytic and green acetylene semihydrogenation processes.In this review,we systematically summarize the recent advances in catalytic technology from thermocatalysis to sustainable alternatives,as well as corresponding regulation strategies for designing high-performance non-noble metal-based catalysts.The crucial factors affecting catalytic performance are discussed,and the fundamental structure-performance correlation of catalysts is outlined.Meanwhile,we emphasize current challenging issues and future perspectives for acetylene semihydrogenation.This review will not only promote the rapid exploration of non-noble metal-based catalysts for acetylene semihydrogenation,but also advance the development of sustainable processes like electrocatalysis and photocatalysis.展开更多
Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structur...Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structures,enriched defects,and unsaturated surface atom coordination.Nevertheless,the manipulation of the amorphous phase in metal-based catalysts is so far impractical,and thus their electrocatalytic mechanism yet remains ambiguous.In this review,the latest advances in AMCs are systematically reviewed,covering amorphous-phase engineering strategy,structure manipulation,and amorphization of various material categories for electrocatalysis.Specifically,a series of applications of AMCs in electrocatalysis for the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),and oxygen evolution reaction(OER)are summarized based on the classification criteria of substances.Finally,we put forward current challenges that have not yet been clarified in the field of AMCs,and propose possible solutions,particularly from the perspective of the evolution of electron microscopy.It is expected to promote the understanding of the amorphization-catalysis relationship and provide a guideline for designing high-performance electrocatalysts.展开更多
Developing lower-cost and higher-effective catalyst to support hydrogen(H_(2))production by electrochemical water-splitting has been recognized as a preferred strategy to drive the clean energy utilization.As a credib...Developing lower-cost and higher-effective catalyst to support hydrogen(H_(2))production by electrochemical water-splitting has been recognized as a preferred strategy to drive the clean energy utilization.As a credible technology for the synthesis of functional materials,electrodeposition has attracted widespread attention,especially suitable for non-noble transition metal-based catalysts(TMCs).Recently,lots of researchers have been devoted to this hot research direction with plentiful achievements,however,a comprehensive review towards this area is still missing.Hence,we summarize the past research progress,presents the technical characteristics of electrodeposition from the viewpoint of fundamental theory and influence factors for the electrochemical deposition behavior,and introduce its application in various of TMCs with versatile nanostructures and compositions.Except a deeper and more comprehensive cognition of electrodeposition,we further discuss the catalyst’s optimized hydrogen evolution reaction(HER),oxygen evolution reaction(OER)performance as well as overall water splitting that combined with the synthetic process.Finally,we conclude the technical advantages towards electrodeposition,propose challenge and future research directions in this promising field.This timely review aims to promote a deeper understanding of effective catalysts obtained via electrodeposition strategy,and provide new guidance for the design and synthesis of future catalysts for hydrogen production.展开更多
The trace amount of CO in H2-rich gas poisons Pt electrode when it is adopted as feedstock for proton-exchange-membrane fuel cells.Preferential oxidation of CO(PROX)is a promising approach to selectively oxidize the t...The trace amount of CO in H2-rich gas poisons Pt electrode when it is adopted as feedstock for proton-exchange-membrane fuel cells.Preferential oxidation of CO(PROX)is a promising approach to selectively oxidize the trace amount of CO while keeping H2 unoxidized.Catalyst plays important roles in PROX.To date,enormous catalysts have been developed for PROX.Summarizing the catalysts developed for PROX and unveiling the reaction mechanism could definitely advance this research field.Herein,in this review,according to the nature of the active sites on the catalysts,we classify the catalysts into group VIII metal-based catalyst,group IB metal-based catalysts,group VIII-group IB bimetallic catalysts,transitional metal oxide catalysts as well as others,describe the progress of the catalysts in PROX in the latest five years,and extract the underlying reaction mechanism,with the aim to provide guidance for the rational design of efficient catalysts in the future.展开更多
The increasing demands of hydrogen and the recent discovery of large reserves of methane have prompted the conversion of methane to hydrogen.The challenges raised by intensive CO_(2) emission from the traditional conv...The increasing demands of hydrogen and the recent discovery of large reserves of methane have prompted the conversion of methane to hydrogen.The challenges raised by intensive CO_(2) emission from the traditional conversion of methane have provoked emission-free hydrogen production from methane.The catalytic decomposition of methane(CDM) to produce hydrogen and advanced carbon hence comes into consideration due to the short process and environmental benignity.Although many researchers have made considerable progress in CDM research on the laboratory scale,CDM is still in its infancy in industrialization.The history of its development,fundamental mechanisms,and recent research progress in catalysts and catalytic systems are herein highlighted.The problems of catalytic interface degradation are reviewed,focusing on deactivation from coke deposition in the CDM process.The introduction of a liquid phase interface which can in-situ remove carbon products provides a new strategy for this process.Furthermore,the challenges and prospects for future research into novel CDM catalysts or catalyst systems are included.展开更多
Alkyne semi-hydrogenation is extremely significant for the production of polymer-grade ethylene and lots of fine chemicals in modem industry.Many efforts had been devoted to regulate the electronic and geometric struc...Alkyne semi-hydrogenation is extremely significant for the production of polymer-grade ethylene and lots of fine chemicals in modem industry.Many efforts had been devoted to regulate the electronic and geometric structure of active ensembles for suppressing side reactions,including over-hydrogenation and oligomerization.Several strategies,such as alloying,surface decoration,atomization of metal centers,and others,were developed to promote the selective production of target alkenes in alkyne hydrogenation.In this review,the basic principles within reaction mechanisms and catalyst optimization would be discussed in detail.And an updated perspective to the fabrication of next-generation catalysts for alkyne semi-hydrogenation is also provided.展开更多
基金supported by the National Natural Science Foundation of China(22202151)Fundamental Research Program of Shanxi Province(202203021212243)。
文摘Ammonia plays an essential role in human production and life as a raw material for chemical fertilizers.The nitrate electroreduction to ammonia reaction(NO_(3)RR)has garnered attention due to its advantages over the Haber-Bosch process and electrochemical nitrogen reduction reaction.Therefore,it represents a promising approach to safeguard the ecological environment by enabling the cycling of nitrogen species.This review begins by discussing the theoretical insights of the NO_(3)RR.It then summarizes recent advances in catalyst design and construction strategies,including alloying,structure engineering,surface engineering,and heterostructure engineering.Finally,the challenges and prospects in this field are presented.This review aims to guide for enhancing the efficiency of electrocatalysts in the NO_(3)RR,and offers insights for converting NO_(3)-to NH_(3).
基金supported by the National Natural Science Foundation of China(22005245,52101271)the Fundamental Research Funds for the Central Universities(G2022KY0606,G2020KY05306,G2022KY05111)+2 种基金Guangdong Basic and Applied Basic Research Foundation(2020A1515111017)the Natural Science Foundation of Shaanxi Province(2021JQ-094)the fellowship of China Postdoctoral Science Foundation(2021M692619)
文摘Selective semihydrogenation of acetylene in raw olefin streams to ethylene is a key industrial reaction to produce polymer-grade feeds for the manufacture of corresponding polymers.The currently used process in industry is the thermocatalytic acetylene semihydrogenation with pressurized hydrogen and Pd-based catalysts at relatively high temperatures.The high cost of Pd urgently desires the design of non-noble metal-based catalysts.However,non-noble metal-based catalysts commonly require much higher reaction temperatures than Pd-based catalysts because of their poor intrinsic activity.Therefore,aiming at increasing economic efficiency and sustainability,various strategies are explored for developing non-noble metal-based catalysts for thermocatalytic and green acetylene semihydrogenation processes.In this review,we systematically summarize the recent advances in catalytic technology from thermocatalysis to sustainable alternatives,as well as corresponding regulation strategies for designing high-performance non-noble metal-based catalysts.The crucial factors affecting catalytic performance are discussed,and the fundamental structure-performance correlation of catalysts is outlined.Meanwhile,we emphasize current challenging issues and future perspectives for acetylene semihydrogenation.This review will not only promote the rapid exploration of non-noble metal-based catalysts for acetylene semihydrogenation,but also advance the development of sustainable processes like electrocatalysis and photocatalysis.
基金the National Natural Science Foundation of China(Nos.52001222,52075361,and U21A20174)the Key National Scientific and Technological Cooperation Projects of Shanxi Province(No.202104041101008)+5 种基金the Major Science and Technology Project of Shanxi Province(No.20201102003)the Key Research and Development Projects in Shanxi Province(No.201903D421030)the Natural Science Foundation of Shanxi Province(Nos.201701D221073 and 201901D111107)the Program for the Innovative Talents of Higher Education Institutions of Shanxi(PTIT)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(STIP,No.2019L025)the Special Foundation for Youth San Jin scholars。
文摘Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structures,enriched defects,and unsaturated surface atom coordination.Nevertheless,the manipulation of the amorphous phase in metal-based catalysts is so far impractical,and thus their electrocatalytic mechanism yet remains ambiguous.In this review,the latest advances in AMCs are systematically reviewed,covering amorphous-phase engineering strategy,structure manipulation,and amorphization of various material categories for electrocatalysis.Specifically,a series of applications of AMCs in electrocatalysis for the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),and oxygen evolution reaction(OER)are summarized based on the classification criteria of substances.Finally,we put forward current challenges that have not yet been clarified in the field of AMCs,and propose possible solutions,particularly from the perspective of the evolution of electron microscopy.It is expected to promote the understanding of the amorphization-catalysis relationship and provide a guideline for designing high-performance electrocatalysts.
基金supported by the National Scientific Foundation of China(Grant No.21878061)。
文摘Developing lower-cost and higher-effective catalyst to support hydrogen(H_(2))production by electrochemical water-splitting has been recognized as a preferred strategy to drive the clean energy utilization.As a credible technology for the synthesis of functional materials,electrodeposition has attracted widespread attention,especially suitable for non-noble transition metal-based catalysts(TMCs).Recently,lots of researchers have been devoted to this hot research direction with plentiful achievements,however,a comprehensive review towards this area is still missing.Hence,we summarize the past research progress,presents the technical characteristics of electrodeposition from the viewpoint of fundamental theory and influence factors for the electrochemical deposition behavior,and introduce its application in various of TMCs with versatile nanostructures and compositions.Except a deeper and more comprehensive cognition of electrodeposition,we further discuss the catalyst’s optimized hydrogen evolution reaction(HER),oxygen evolution reaction(OER)performance as well as overall water splitting that combined with the synthetic process.Finally,we conclude the technical advantages towards electrodeposition,propose challenge and future research directions in this promising field.This timely review aims to promote a deeper understanding of effective catalysts obtained via electrodeposition strategy,and provide new guidance for the design and synthesis of future catalysts for hydrogen production.
基金support from the National Natural Science Foundation of China(No.21902116)the Scientific Research Foundation of Liaoning province of China(No.JQL202015403).
文摘The trace amount of CO in H2-rich gas poisons Pt electrode when it is adopted as feedstock for proton-exchange-membrane fuel cells.Preferential oxidation of CO(PROX)is a promising approach to selectively oxidize the trace amount of CO while keeping H2 unoxidized.Catalyst plays important roles in PROX.To date,enormous catalysts have been developed for PROX.Summarizing the catalysts developed for PROX and unveiling the reaction mechanism could definitely advance this research field.Herein,in this review,according to the nature of the active sites on the catalysts,we classify the catalysts into group VIII metal-based catalyst,group IB metal-based catalysts,group VIII-group IB bimetallic catalysts,transitional metal oxide catalysts as well as others,describe the progress of the catalysts in PROX in the latest five years,and extract the underlying reaction mechanism,with the aim to provide guidance for the rational design of efficient catalysts in the future.
基金the funding support from the National Natural Science Foundation of China(51722404,51674177,51804221 and 91845113)the National Key R&D Program of China(2018YFE0201703)+2 种基金the China Postdoctoral Science Foundation(2018M642906 and 2019T120684)the Fundamental Research Funds for the Central Universities(2042019kf0230)the Hubei Provincial Natural Science Foundation of China(2019CFA065)。
文摘The increasing demands of hydrogen and the recent discovery of large reserves of methane have prompted the conversion of methane to hydrogen.The challenges raised by intensive CO_(2) emission from the traditional conversion of methane have provoked emission-free hydrogen production from methane.The catalytic decomposition of methane(CDM) to produce hydrogen and advanced carbon hence comes into consideration due to the short process and environmental benignity.Although many researchers have made considerable progress in CDM research on the laboratory scale,CDM is still in its infancy in industrialization.The history of its development,fundamental mechanisms,and recent research progress in catalysts and catalytic systems are herein highlighted.The problems of catalytic interface degradation are reviewed,focusing on deactivation from coke deposition in the CDM process.The introduction of a liquid phase interface which can in-situ remove carbon products provides a new strategy for this process.Furthermore,the challenges and prospects for future research into novel CDM catalysts or catalyst systems are included.
基金Financial support from the National Key Research and Development Program of China(No.2021YFB3801600)the National Natural Science Foundation of China(Nos.21872121 and 21908189)the“Pioneer”and“Leading Goose”R&D Program of Zhejiang Province(Nos.2022C01218 and 2022C01151)are greatly appreciated.
文摘Alkyne semi-hydrogenation is extremely significant for the production of polymer-grade ethylene and lots of fine chemicals in modem industry.Many efforts had been devoted to regulate the electronic and geometric structure of active ensembles for suppressing side reactions,including over-hydrogenation and oligomerization.Several strategies,such as alloying,surface decoration,atomization of metal centers,and others,were developed to promote the selective production of target alkenes in alkyne hydrogenation.In this review,the basic principles within reaction mechanisms and catalyst optimization would be discussed in detail.And an updated perspective to the fabrication of next-generation catalysts for alkyne semi-hydrogenation is also provided.
