Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites
2020-04-17
发表期刊ACS CATALYSIS
ISSN21555435
卷号10期号:8页码:4534-4542
发表状态已发表
DOI10.1021/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.
© 2020 American Chemical Society.

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 CO2 Reduction: Operando Diagnosis of Active Sites[J]. ACS CATALYSIS,2020,10(8):4534-4542.
APA Ma, Lushan.,Hu, Weibo.,Mei, Bingbao.,Liu, Hong.,Yuan, Biao.,...&Yang, Hui.(2020).Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites.ACS CATALYSIS,10(8),4534-4542.
MLA Ma, Lushan,et al."Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites".ACS CATALYSIS 10.8(2020):4534-4542.
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