Bioinspired iron porphyrins with appended poly-pyridine/amine units for boosted electrocatalytic CO2 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

eScience (Nov 2022)

Bioinspired iron porphyrins with appended poly-pyridine/amine units for boosted electrocatalytic CO2 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

Affiliations

Jinxiu Han: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Ni Wang: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Xialiang Li: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Haitao Lei: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Yabo Wang: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Hongbo Guo: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Xiaotong Jin: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Qingxin Zhang: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Xinyang Peng: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Xue-Peng Zhang: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China; Corresponding authors.
Wei Zhang: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China
Ulf-Peter Apfel: Ruhr-Universität Bochum, Fakultät für Chemie und Biochemie, Anorganische Chemie I Universitätsstrasse 150, 44801, Bochum, Germany; Fraunhofer UMSICHT, Department for Electrosynthesis, 46047, Oberhausen, Germany
Rui Cao: Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China; Corresponding authors.

Journal volume & issue: Vol. 2, no. 6
pp. 623 – 631

Abstract

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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-to-CO 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 TOFmax 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.

Published in eScience

ISSN: 2667-1417 (Online)
Publisher: KeAi Communications Co. Ltd.
Country of publisher: China
LCC subjects: Technology: Mechanical engineering and machinery; Technology: Electrical engineering. Electronics. Nuclear engineering: Electronics
Website: https://www.keaipublishing.com/en/journals/escience/

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