Metal-like behavior of a 2D molecular catalyst enables redox-decoupled electrocatalysis.

Yang Wang, Dongyu Zhang, Ting Chen, Caijie Su, Yi Xie, Changzheng Wu, Nikolay Kornienko

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Article in National science review, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.

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7 authors.

Yang WangState Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei 230026, China.

Dongyu ZhangDepartment of Chemical Engineering and Chemistry, Eindhoven University of Technology, Eindhoven 5612 AE, The Netherlands.

Ting ChenState Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei 230026, China.

Caijie SuState Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei 230026, China.

Yi XieState Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei 230026, China.

Changzheng WuState Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei 230026, China.

Nikolay KornienkoInstitute of Inorganic Chemistry, Department of Chemistry, University of Bonn, Bonn 53121, Germany.ORCID https://orcid.org/0000-0001-7193-2428

Funding

No grant is acknowledged in the PubMed record.

6 · The paper itself

Abstract

Molecular catalysts facilitate electrochemical conversion by changing their oxidation states to transfer electrons. However, this redox-mediated mechanism features stepwise electron transfer and substrate activation in separate elementary steps, thereby resulting in an inherent loss in efficiency. Here, we synthesize a two-dimensional (2D) iron phthalocyanine (FePc) material and uncover its non-mediated electron transfer behavior in electrocatalysis, which overcomes the conventional redox-mediated limitation in the oxygen reduction reaction (ORR) pathway that molecular catalysts face. The 2D geometry enables the FePc molecules to be positioned within the electrochemical double layer, enabling electrons to directly transfer to oxygen reactants, prior to the Fe(II/III) redox. This functions in a manner akin to a metal catalyst thereby opening a redox-decoupled ORR mechanism. As a result, the reported 2D FePc molecular catalyst exhibits unprecedented ORR half-wave potential at 0.945 V vs. the reversible hydrogen electrode, achieving efficient application in zinc-air batteries and H

Indexed as

fuel cellsmetal-like electron transfer behaviormolecular catalystoxygen reduction reactionredox-decoupled mechanismtwo-dimensional confinement

Identifiers

PMID40635686

DOI10.1093/nsr/nwaf198

PMCPMC12236314

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