摘要
可再生能源驱动电催化二氧化碳还原制备高附加值化学燃料,是一种实现二氧化碳资源化的有效途径.以金属有机骨架(MOF)为模板制备的层状双金属氢氧化物空心多面体已成为当前电催化领域的热门材料.然而,该类材料的高析氢活性严重阻碍了其在电催化二氧化碳还原中的应用.基于此,本文报道了一种在离子液体电解液中可高效稳定电催化二氧化碳还原的钴铁层状双金属氢氧化物空心多面体(CoFe LDH/HP),其最大法拉第转换效率可达86%±3%(-0.9 V相对于可逆氢电极),且可连续电解30 h.实验结果表明此CoFe LDH/HP因其独特的空心结构可暴露更多的活性位点,从而具有更快的电催化二氧化碳还原动力学;理论计算表明CoFe LDH/HP中Co-O-Fe键有利于稳定关键中间体(*COOH)并降低相应的活化势垒.本研究可为其他层状双金属氢氧化物用于二氧化碳固定的设计提供参考.
Over the past several decades,the utilization of fossil fuels is responsible for mainly excessive atmospheric carbon dioxide(CO_(2))[1-3].Increased concentration of CO_(2)contributes to the major portion of the critical issues faced worldwide,such as global warming and drastic changes in climate.Therefore,it is imperative to develop an alternative technology that is capable of providing an efficient and sustainable pathway to target the neutralization of CO_(2)level in the atmosphere.
作者
杨淼森
孙甲强
秦永吉
杨慧
张书胜
刘熙俊
罗俊
Miaosen Yang;Jiaqiang Sun;Yongji Qin;Hui Yang;Shusheng Zhang;Xijun Liu;Jun Luo(School of Chemical Engineering,Northeast Electric Power University,Jilin 132012,China;Nanchang Institute of Technology,Nanchang 330044,China;State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;Institute for New Energy Materials and Low-Carbon Technologies,Tianjin Key Lab for Photoelectric Materials&Devices,School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China;School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China;College of Chemistry,Zhengzhou University,Zhengzhou 450000,China;MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials,and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials,School of Physical Science and Technology,Guangxi University,Nanning 530004,China)
基金
supported by the Research Fund of State Key Laboratory for Marine Corrosion and Protection of Luoyang Ship Material Research Institute(LSMRI)(KF190411)
Tianjin Natural Science Foundation(18JCQNJC77100)
Beijing PARATERA Tech CO.,Ltd.for providing HPC resources that have contributed to the research results reported in this paper。
