Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites
文献类型：期刊论文
| 作者 | Ma, LS; Hu, WB; Mei, BB; Liu, H; Yuan, B; Zang, J; Chen, T; Zou, LL; Zou, ZQ; Yang, B |
| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2020 |
| 卷号 | 10期号:8页码:4534-4542 |
| 关键词 | CARBON-DIOXIDE ELECTROREDUCTION HYDROCARBONS COVERAGE ELECTROCATALYSTS MULTICARBON CHALLENGES ELECTRODES EFFICIENCY CONVERSION |
| ISSN号 | 2155-5435 |
| DOI | 10.1021/acscatal.0c00243 |
| 文献子类 | 期刊论文 |
| 英文摘要 | 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 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. |
| 语种 | 英语 |
| 源URL | [http://ir.sinap.ac.cn/handle/331007/32771]  |
| 专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
| 作者单位 | 1.Univ Chinese Acad Sci, Beijing 100039, Peoples R China 2.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China 3.Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 4.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：上海应用物理研究所
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