Cadmium-based metal-organic frameworks for high-performance electrochemical CO2 reduction to CO over wide potential range

doi:10.1016/j.cjche.2021.10.013

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 143-151.DOI: 10.1016/j.cjche.2021.10.013

Cadmium-based metal-organic frameworks for high-performance electrochemical CO₂ reduction to CO over wide potential range

Xin Li¹, Song Hong², Leiduan Hao¹, Zhenyu Sun¹

1. State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China;
2. College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China

收稿日期:2021-06-30 修回日期:2021-09-12 出版日期:2022-03-28 发布日期:2022-04-28
通讯作者: Zhenyu Sun,E-mail:sunzy@mail.buct.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (No. 21972010); Beijing Natural Science Foundation (No. 2192039); Beijing University of Chemical Technology (XK180301), and the Foundation of Key Laboratory of Low-Carbon Conversion Science & Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences (No. KLLCCSE-201901, SARI, CAS).

Cadmium-based metal-organic frameworks for high-performance electrochemical CO₂ reduction to CO over wide potential range

Xin Li¹, Song Hong², Leiduan Hao¹, Zhenyu Sun¹

1. State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China;
2. College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China

Received:2021-06-30 Revised:2021-09-12 Online:2022-03-28 Published:2022-04-28
Contact: Zhenyu Sun,E-mail:sunzy@mail.buct.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (No. 21972010); Beijing Natural Science Foundation (No. 2192039); Beijing University of Chemical Technology (XK180301), and the Foundation of Key Laboratory of Low-Carbon Conversion Science & Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences (No. KLLCCSE-201901, SARI, CAS).

摘要/Abstract

摘要： Electrochemical CO₂ reduction (ECR) powered by renewable energy sources provides a sustainable avenue to producing carbon–neutral fuels and chemicals. The design and development of high performance, cost-effective, and stable catalysts for ECR remain a focus of intense research. Here, we report a novel electrocatalyst, two-dimensional cadmium-based 1,4-benzenedicarboxylate metal–organic frameworks (Cd-BDC MOFs) which can effectively convert CO₂ to CO with a faradaic efficiency (FE) of more than 80.0% over the voltage range between -0.9 and -1.1 V (versus reversible hydrogen electrode, vs. RHE) in 0.1 mol·L^-1 CO₂-saturated KHCO₃ solution with an H-type cell, reaching up to 88.9% at -1.0 V (vs. RHE). The performance outperforms commercial CdO and many other MOF-based materials demonstrated in prior literature. The catalytic property can be readily tuned by manipulating synthesis conditions as well as electrolyte type. Especially, high CO FEs exceeding 90.0% can be attained on the Cd-BDC electrode at potentials ranging from -0.16 to -1.06 V (vs. RHE) in 0.5 mol·L^-1 KHCO₃ solution by using a gas diffusion electrode cell system. The maximum CO FE approaches ~97.6% at -0.26 V (vs. RHE) and the CO partial geometric current density is as high as about 108.1 mA cm^-2 at -1.1 V (vs. RHE). This work offers an efficient, low cost, and alternative electrocatalyst for CO₂ transformation.

关键词: Electrochemical carbon dioxide reduction, Carbon monoxide, Cadmium, Metal-organic framework, Electrocatalysis

Abstract: Electrochemical CO₂ reduction (ECR) powered by renewable energy sources provides a sustainable avenue to producing carbon–neutral fuels and chemicals. The design and development of high performance, cost-effective, and stable catalysts for ECR remain a focus of intense research. Here, we report a novel electrocatalyst, two-dimensional cadmium-based 1,4-benzenedicarboxylate metal–organic frameworks (Cd-BDC MOFs) which can effectively convert CO₂ to CO with a faradaic efficiency (FE) of more than 80.0% over the voltage range between -0.9 and -1.1 V (versus reversible hydrogen electrode, vs. RHE) in 0.1 mol·L^-1 CO₂-saturated KHCO₃ solution with an H-type cell, reaching up to 88.9% at -1.0 V (vs. RHE). The performance outperforms commercial CdO and many other MOF-based materials demonstrated in prior literature. The catalytic property can be readily tuned by manipulating synthesis conditions as well as electrolyte type. Especially, high CO FEs exceeding 90.0% can be attained on the Cd-BDC electrode at potentials ranging from -0.16 to -1.06 V (vs. RHE) in 0.5 mol·L^-1 KHCO₃ solution by using a gas diffusion electrode cell system. The maximum CO FE approaches ~97.6% at -0.26 V (vs. RHE) and the CO partial geometric current density is as high as about 108.1 mA cm^-2 at -1.1 V (vs. RHE). This work offers an efficient, low cost, and alternative electrocatalyst for CO₂ transformation.

Key words: Electrochemical carbon dioxide reduction, Carbon monoxide, Cadmium, Metal-organic framework, Electrocatalysis

Xin Li, Song Hong, Leiduan Hao, Zhenyu Sun. Cadmium-based metal-organic frameworks for high-performance electrochemical CO₂ reduction to CO over wide potential range[J]. 中国化学工程学报, 2022, 43(3): 143-151.

Xin Li, Song Hong, Leiduan Hao, Zhenyu Sun. Cadmium-based metal-organic frameworks for high-performance electrochemical CO₂ reduction to CO over wide potential range[J]. Chinese Journal of Chemical Engineering, 2022, 43(3): 143-151.

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Cadmium-based metal-organic frameworks for high-performance electrochemical CO₂ reduction to CO over wide potential range

Cadmium-based metal-organic frameworks for high-performance electrochemical CO₂ reduction to CO over wide potential range

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