Bioinspired iron porphyrins with appended polypyridine/amine units for boosted electrocatalytic CO<sub>2</sub> reduction reaction

Jinxiu Han; Ni Wang; Xialiang Li; Haitao Lei; Yabo Wang; Hongbo Guo; Xiaotong Jin; Qingxin Zhang; Xinyang Peng; Xue-Peng Zhang; Wei Zhang; Ulf-Peter Apfel; Rui Cao

doi:10.1016/j.esci.2022.06.003

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Jinxiu Han, Ni Wang, Xialiang Li, Haitao Lei, Yabo Wang, Hongbo Guo, Xiaotong Jin, Qingxin Zhang, Xinyang Peng, Xue-Peng Zhang, Wei Zhang, Ulf-Peter Apfel, Rui Cao. Bioinspired iron porphyrins with appended polypyridine/amine units for boosted electrocatalytic CO2 reduction reaction[J]. eScience. doi: 10.1016/j.esci.2022.06.003

Citation:

Jinxiu Han, Ni Wang, Xialiang Li, Haitao Lei, Yabo Wang, Hongbo Guo, Xiaotong Jin, Qingxin Zhang, Xinyang Peng, Xue-Peng Zhang, Wei Zhang, Ulf-Peter Apfel, Rui Cao. Bioinspired iron porphyrins with appended polypyridine/amine units for boosted electrocatalytic CO₂ reduction reaction[J]. eScience. doi: 10.1016/j.esci.2022.06.003

Citation:

Jinxiu Han, Ni Wang, Xialiang Li, Haitao Lei, Yabo Wang, Hongbo Guo, Xiaotong Jin, Qingxin Zhang, Xinyang Peng, Xue-Peng Zhang, Wei Zhang, Ulf-Peter Apfel, Rui Cao. Bioinspired iron porphyrins with appended polypyridine/amine units for boosted electrocatalytic CO₂ reduction reaction[J]. eScience. doi: 10.1016/j.esci.2022.06.003

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Bioinspired iron porphyrins with appended polypyridine/amine units for boosted electrocatalytic CO₂ reduction reaction

doi: 10.1016/j.esci.2022.06.003

1 Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an 710119, China;
2 Ruhr-Universität Bochum, Fakultät für Chemie und Biochemie, Anorganische Chemie I Universitätsstrasse 150, 44801 Bochum, Germany;
3 Fraunhofer UMSICHT, Department for Electrosynthesis, 46047 Oberhausen, Germany

Received Date: 2022-03-17
Revised Date: 2022-05-20
Accepted Date: 2022-06-11

Available Online: 2022-06-23

Abstract

Abstract

Developing highly efficient electrocatalysts for the CO₂ reduction reaction (CO₂RR) has attracted increasing interest in the past decade. Herein, we report on the design and synthesis of Fe porphyrin 1 with an appended N,N-di(2- picolyl)ethylenediamine (DPEN) unit that boosts electrocatalytic activity for CO₂-toCO conversion in acetonitrile with water as the proton source. By mimicking carbon monoxide dehydrogenase (CODH), 1 has poly-pyridine/amine units located at the active site to form hydrogen-bonded water-containing networks that enable fast proton transfer. The protonated and positively charged DPEN unit can also stabilize CO₂ reduction intermediates through electrostatic and hydrogen-bonding interactions. These factors make 1 a highly active electrocatalyst for the CO₂RR by achieving a TOF_max of 5.0 × 10⁴ s⁻¹ with water providing the protons. These critical roles of the DPEN unit in the CO₂RR are further supported by theoretical studies. This work is significant to highlight the benefits of using molecular catalysts to elucidate structural effects.
- CO₂ reduction reaction,
- Fe porphyrin,
- Molecular electrocatalysis,
- Structural effect,
- Water network

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We are grateful for support from National Natural Science Foundation of China (21773146, 22003036 and 22171176), Fok Ying-Tong Education Foundation for Outstanding Young Teachers in University, Fundamental Research Funds for the Central Universities (GK202103045 and GK202103033), the Research Funds of Shaanxi Normal University, and the open fund of State Key Laboratory of Structural Chemistry. U.-P. A. thanks for the support by the Fraunhofer Internal Programs under Grant No. Attract 097-602175 and the DFG under Germany’s Excellence StrategyEXC-2033-Projektnummer 390677874 "RESOLV".

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