Fourteen-membered macrocyclic cobalt complex for the electrolysis of low-concentration gaseous carbon dioxide with high faradaic efficiency toward carbon monoxide

Takeshi Inada; Shoji Iguchi; Masahiro Yamamoto; Yusuke Hasegawa; Makoto Moriya; Junya Ohyama; Yuta Nabae; Shimpei Naniwa; Tsunehiro Tanaka; Kentaro Teramura

doi:10.1039/D3CY01177A

Fourteen-membered macrocyclic cobalt complex for the electrolysis of low-concentration gaseous carbon dioxide with high faradaic efficiency toward carbon monoxide†

Takeshi Inada,^a Shoji Iguchi,

*^a Masahiro Yamamoto,^a Yusuke Hasegawa,^a Makoto Moriya,

^bc Junya Ohyama,

^d Yuta Nabae,

^e Shimpei Naniwa,

^a Tsunehiro Tanaka

^afg and Kentaro Teramura

*^afg

Author affiliations

* Corresponding authors

^a Graduate School of Engineering, Kyoto University, Kyoto daigaku-katsura, Nishikyo-ku, Kyoto 615-8530, Japan
E-mail: iguchi.shoji.4k@kyoto-u.ac.jp, teramura.kentaro.7r@kyoto-u.ac.jp

^b College of Science, Academic Institute, Shizuoka University, 836, Ohya, Suruga-ku, Shizuoka 422-8529, Japan

^c Research Institute of Green Science and Technology, Shizuoka University, 836 Ohya, Suruga-ku, Shizuoka 422-8529, Japan

^d Faculty of Advanced Science and Technology, Kumamoto University, 2-39-1 Kurokami, Chuo-ku, Kumamoto 860-8555, Japan

^e Department of Materials Science and Engineering, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8552, Japan

^f Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan

^g Fukui Institute for Fundamental Chemistry (FIFC), Kyoto University, 34-4 Takano-Nishibiraki-cho, Sakyou-ku, Kyoto 606-8103, Japan

Abstract

It is necessary to lower the overpotential for CO₂ reduction to enable the practical application of CO₂ electrolysis in industrial scenarios. In gaseous CO₂ electrolysis with a gas diffusion electrode, a fourteen-membered macrocyclic cobalt complex (Co 14-membered ring: Co–14MR) was found to be an excellent cathode catalyst for the reduction of CO₂ to CO. A high current density (101 mA cm⁻² at −2.05 V (Ag/AgCl)), high faradaic efficiency (>99%), low overpotential (onset potential of CO formation: −0.13 V (RHE)), and high durability (stable performance until turn over number (TON) = 2.3 × 10⁴ per Co atom) were achieved. Moreover, CO was generated with a faradaic efficiency of 95% during CO₂ electrolysis with the Co–14MR cathode under a low CO₂ concentration (10% CO₂). The single-atom Co site in the Co–14MR catalyst enabled the near-complete suppression of undesired H₂ evolution.

Catalysis Science & Technology

Fourteen-membered macrocyclic cobalt complex for the electrolysis of low-concentration gaseous carbon dioxide with high faradaic efficiency toward carbon monoxide†

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Fourteen-membered macrocyclic cobalt complex for the electrolysis of low-concentration gaseous carbon dioxide with high faradaic efficiency toward carbon monoxide

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