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Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO | |
2020-04-17 | |
发表期刊 | ACS CATALYSIS |
ISSN | 21555435 |
卷号 | 10期号:8页码:4534-4542 |
发表状态 | 已发表 |
DOI | 10.1021/acscatal.0c00243 |
摘要 | Developing efficient catalysts for steering the electrochemical CO2 reduction reaction (CO2RR) toward high-value chemicals beyond CO and formic acid is highly desirable. Herein, we have developed copper-based catalysts confined within a rationally designed covalent triazine framework (CTF-B), featuring a CuN2Cl2 structure, for selective CO2RR to hydrocarbons with a maximum Faradaic efficiency (FE) of 81.3% and an FE of C2H4 up to 30.6%. Operando X-ray adsorption fine structure analyses reveal the potential-driven dynamic formation of Cu atomic clusters, together with the time-dependent and Cu-content-dependent CO2RR performance associated with the catalyst activation, definitively uncovering that the aggregated Cu clusters confined within CTF-B are the active sites. A further probing experiment of CO electroreduction not only verifies that CO is one of the key intermediates for the CO2RR but also demonstrates the improved selectivity to C2 chemicals, with a maximum FE of 68.4% (C2H4, 35.0%; acetate, 33.4%), possibly originating from the accelerative C-C coupling reaction due to the increased CO coverage and enhanced local pH in CO-saturated electrolyte. Interestingly, acetate is identified as the only liquid product, mostly likely benefiting from the dominant low-coordination active sites of confined Cu aggregation and favorable chemical confinement environment of CTF-B. The strategy of constructing efficient metalloelectrocatalysts by means of confinement in a covalent organic framework along with operando identification of active sites sheds light on the rational catalyst design and structure-property relationship. |
收录类别 | SCI ; SCIE ; EI |
语种 | 英语 |
资助项目 | National Key Research and Development Programs of China[2017YFA0206500] ; National Natural Science Foundation of China[21902176][21872165] ; DNL Cooperation Fund, CAS[DNL201924] |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Physical |
出版者 | American Chemical Society |
EI入藏号 | 20202008665428 |
EI主题词 | Carbon dioxide ; Catalyst activity ; Chemical bonds ; Chlorine compounds ; Copper compounds ; Electrolytes ; Electrolytic reduction ; Ethylene ; Reaction intermediates |
EI分类号 | Ore Treatment:533.1 ; Copper:544.1 ; Physical Chemistry:801.4 ; Chemical Products Generally:804 |
WOS关键词 | CARBON-DIOXIDE ; ELECTROREDUCTION ; HYDROCARBONS ; COVERAGE ; ELECTROCATALYSTS ; MULTICARBON ; CHALLENGES ; ELECTRODES ; EFFICIENCY ; CONVERSION |
原始文献类型 | Article |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/121554 |
专题 | 物质科学与技术学院_硕士生 物质科学与技术学院_PI研究组_杨波组 物质科学与技术学院_特聘教授组_文珂组 物质科学与技术学院_特聘教授组_杨辉组 物质科学与技术学院_PI研究组_于奕组 物质科学与技术学院_博士生 |
通讯作者 | Zou, Liangliang; Yang, Hui |
作者单位 | 1.Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai; 201210, China 2.University of Chinese Academy of Sciences, Beijing; 100039, China 3.Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Dalian; 116023, China 4.Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai; 201210, China 5.School of Physical Science and Technology, ShanghaiTech University, Shanghai; 201210, China |
推荐引用方式 GB/T 7714 |
Ma, Lushan,Hu, Weibo,Mei, Bingbao,et al. Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO |
APA |
Ma, Lushan.,Hu, Weibo.,Mei, Bingbao.,Liu, Hong.,Yuan, Biao.,...&Yang, Hui.(2020).Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO |
MLA |
Ma, Lushan,et al."Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO |
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