CAS OpenIR  > 中科院上海应用物理研究所2011-2020年
Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites
Ma, LS; Hu, WB; Mei, BB; Liu, H; Yuan, B; Zang, J; Chen, T; Zou, LL; Zou, ZQ; Yang, B; Yu, Y; Ma, JY; Jiang, Z; Wen, K; Yang, H
2020
Source PublicationACS CATALYSIS
ISSN2155-5435
Volume10Issue:8Pages:4534-4542
Subtype期刊论文
AbstractDeveloping 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 C-2 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.
KeywordCARBON-DIOXIDE ELECTROREDUCTION HYDROCARBONS COVERAGE ELECTROCATALYSTS MULTICARBON CHALLENGES ELECTRODES EFFICIENCY CONVERSION
DOI10.1021/acscatal.0c00243
Indexed BySCI
Language英语
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Cited Times:18[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/32771
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
2.Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100039, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China
5.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
Recommended Citation
GB/T 7714
Ma, LS,Hu, WB,Mei, BB,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, LS.,Hu, WB.,Mei, BB.,Liu, H.,Yuan, B.,...&Yang, H.(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, LS,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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