Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO2 reduction to formate

doi:10.1016/j.cjche.2022.03.006

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 353-359.DOI: 10.1016/j.cjche.2022.03.006

Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO₂ reduction to formate

Yachen Deng, Shifu Wang, Yanqiang Huang, Xuning Li

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

收稿日期:2022-02-25 修回日期:2022-03-13 出版日期:2022-03-28 发布日期:2022-04-28
通讯作者: Xuning Li,E-mail:lixn@dicp.ac.cn
基金资助:
This work was financially supported by the National Key Research and Development Program of China (No. 2021YFA1500502), the National Natural Science Foundation of China (22102176), CAS Project for Young Scientists in Basic Research (YSBR-022) and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB36030200).

Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO₂ reduction to formate

Yachen Deng, Shifu Wang, Yanqiang Huang, Xuning Li

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

Received:2022-02-25 Revised:2022-03-13 Online:2022-03-28 Published:2022-04-28
Contact: Xuning Li,E-mail:lixn@dicp.ac.cn
Supported by:
This work was financially supported by the National Key Research and Development Program of China (No. 2021YFA1500502), the National Natural Science Foundation of China (22102176), CAS Project for Young Scientists in Basic Research (YSBR-022) and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB36030200).

摘要/Abstract

摘要： MOF-based materials have been widely explored in electrochemical CO₂ reduction reactions for the production of valuable chemicals. Understanding the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction mechanism. Herein, a series of six N coordinated Sn-based metal-organic frameworks (Sn-N6-MOFs) are newly developed for electrochemical CO₂ reduction (CO₂RR). 2% Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of ~85% and a current density of 23 mA·cm^-2 at -1.23 V vs. RHE. In-situ Raman results combined with ex-situ ¹¹⁹Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO₂RR, generating tin nanoclusters as the real active sites for CO₂ electroreduction to HCOOH.

关键词: Structural reconstruction, Metal-organic frameworks, Mössbauer spectroscopy, Electrochemical CO₂ reduction

Abstract: MOF-based materials have been widely explored in electrochemical CO₂ reduction reactions for the production of valuable chemicals. Understanding the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction mechanism. Herein, a series of six N coordinated Sn-based metal-organic frameworks (Sn-N6-MOFs) are newly developed for electrochemical CO₂ reduction (CO₂RR). 2% Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of ~85% and a current density of 23 mA·cm^-2 at -1.23 V vs. RHE. In-situ Raman results combined with ex-situ ¹¹⁹Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO₂RR, generating tin nanoclusters as the real active sites for CO₂ electroreduction to HCOOH.

Key words: Structural reconstruction, Metal-organic frameworks, Mössbauer spectroscopy, Electrochemical CO₂ reduction

Yachen Deng, Shifu Wang, Yanqiang Huang, Xuning Li. Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO₂ reduction to formate[J]. 中国化学工程学报, 2022, 43(3): 353-359.

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Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO₂ reduction to formate

Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO₂ reduction to formate

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