With the rapid development of economy,the consumption of fossil fuels and excessive emissions of carbon dioxide(CO_(2))have led to many environmental issues.The thermocatalytic conversion of CO_(2) to high value‐adde...With the rapid development of economy,the consumption of fossil fuels and excessive emissions of carbon dioxide(CO_(2))have led to many environmental issues.The thermocatalytic conversion of CO_(2) to high value‐added chemicals is an effective strategy to meet the need of carbon neutralization.Among them,CO_(2) hydrogenation to light olefins has been well researched so that the selectivity of desired products can exceed the Anderson–Schulz–Flory(ASF)distribution to acquire an extremely high yield.However,although huge progress has been made in CO_(2) hydrogenation to produce long‐chainα‐olefins based on Fe catalysts as well,designing efficient catalysts with promoted C‐O dissociation and C‐C coupling remains challenging.In addition,ASF distribution restrains the selectivity of desired long‐chain products,whereas the approaches to breaking it still face issues.In this review,we focus on the design of Fe‐based catalysts for the synthesis of long‐chainα‐olefins through CO_(2) hydrogenation.We have summarized and analyzed the reaction mechanism,design of catalysts,structure–activity relationship,interaction between Fe and promoters,and strategies to break the ASF distribution.At the same time,the issues faced by CO_(2) hydrogenation to long‐chainα‐olefins are proposed and the possible future solutions are prospected.This review aims to provide a recent development on the design of Fe‐based catalysts for CO_(2) hydrogenation to long‐chainα‐olefins while considering the ASF distribution.展开更多
The performance of asymmetric supercapacitors(ASCs)is strongly restricted by the capacity gap between the positive and negative electrodes.To address this issue,two new electrode materials deriving from Co‐and Fe‐ba...The performance of asymmetric supercapacitors(ASCs)is strongly restricted by the capacity gap between the positive and negative electrodes.To address this issue,two new electrode materials deriving from Co‐and Fe‐based metal–organic frameworks(MOFs,Co‐TAMBA‐d,and Fe‐TAMBA‐d)through a single‐step sintering method have been developed by considering the superiorities of the derivatives of MOFs including large surface areas,sufficient metal‐atom‐doping content,and extreme surface wettability to the bath solution.The as‐prepared Co‐TAMBA‐d as a positive electrode delivers typical pseudocapacitive behavior with the improvement of capacity,which is better than those of pristine MOF materials,while Fe‐TAMBA‐d as negative electrodes displays better electrochemical behavior than those of activated carbon.ASCs based on these two electrodes exhibits excellent energy density and power density of 47Wh/kg and 1658 W/kg,respectively,where this device can maintain prominent cycling stability with capacity retention after 5000 cycles being about 75%.Furthermore,the capacity can feed a series of red light‐emitting diodes,which gives solid evidence of the potential utilization.These results can afford the feasibility of isostructural MOF derivatives as promising electrodes in novel ASCs.展开更多
基金supported by the CNPC Innovation Found(2021DQ02‐0702).
文摘With the rapid development of economy,the consumption of fossil fuels and excessive emissions of carbon dioxide(CO_(2))have led to many environmental issues.The thermocatalytic conversion of CO_(2) to high value‐added chemicals is an effective strategy to meet the need of carbon neutralization.Among them,CO_(2) hydrogenation to light olefins has been well researched so that the selectivity of desired products can exceed the Anderson–Schulz–Flory(ASF)distribution to acquire an extremely high yield.However,although huge progress has been made in CO_(2) hydrogenation to produce long‐chainα‐olefins based on Fe catalysts as well,designing efficient catalysts with promoted C‐O dissociation and C‐C coupling remains challenging.In addition,ASF distribution restrains the selectivity of desired long‐chain products,whereas the approaches to breaking it still face issues.In this review,we focus on the design of Fe‐based catalysts for the synthesis of long‐chainα‐olefins through CO_(2) hydrogenation.We have summarized and analyzed the reaction mechanism,design of catalysts,structure–activity relationship,interaction between Fe and promoters,and strategies to break the ASF distribution.At the same time,the issues faced by CO_(2) hydrogenation to long‐chainα‐olefins are proposed and the possible future solutions are prospected.This review aims to provide a recent development on the design of Fe‐based catalysts for CO_(2) hydrogenation to long‐chainα‐olefins while considering the ASF distribution.
基金National Natural Science Foundation of China,Grant/Award Numbers:22279061,21901120,21371098The Fundamental Research Funds for the Central Universities,the Natural Science Foundation of Jiangsu Province,Grant/Award Numbers:BK20180514,BK20190503,BK20131314+1 种基金The Qing Lan Project of Jiangsu Province.Q.Z.thanks the funding support from City University of Hong Kong,Grant/Award Numbers:9380117,7005620 and 7020040Hong Kong Institute for Advanced Study,City University of Hong Kong,China。
文摘The performance of asymmetric supercapacitors(ASCs)is strongly restricted by the capacity gap between the positive and negative electrodes.To address this issue,two new electrode materials deriving from Co‐and Fe‐based metal–organic frameworks(MOFs,Co‐TAMBA‐d,and Fe‐TAMBA‐d)through a single‐step sintering method have been developed by considering the superiorities of the derivatives of MOFs including large surface areas,sufficient metal‐atom‐doping content,and extreme surface wettability to the bath solution.The as‐prepared Co‐TAMBA‐d as a positive electrode delivers typical pseudocapacitive behavior with the improvement of capacity,which is better than those of pristine MOF materials,while Fe‐TAMBA‐d as negative electrodes displays better electrochemical behavior than those of activated carbon.ASCs based on these two electrodes exhibits excellent energy density and power density of 47Wh/kg and 1658 W/kg,respectively,where this device can maintain prominent cycling stability with capacity retention after 5000 cycles being about 75%.Furthermore,the capacity can feed a series of red light‐emitting diodes,which gives solid evidence of the potential utilization.These results can afford the feasibility of isostructural MOF derivatives as promising electrodes in novel ASCs.
