Soluble Gd6Cu24 clusters: effective molecular electrocatalysts for water oxidation

Jia-Nan Chen; Zhong-Hua Pan; Qi-Hao Qiu; Cheng Wang; La-Sheng Long; Lan-Sun Zheng; Xiang-Jian Kong

doi:10.1039/D3SC05849B

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Soluble Gd₆Cu₂₄ clusters: effective molecular electrocatalysts for water oxidation†

Jia-Nan Chen,‡^a Zhong-Hua Pan,‡^a Qi-Hao Qiu,^a Cheng Wang,

^a La-Sheng Long,

^a Lan-Sun Zheng^a and Xiang-Jian Kong

*^a

Author affiliations

* Corresponding authors

^a Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory of Physical Chemistry of Solid Surface, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China
E-mail: xjkong@xmu.edu.cn

Abstract

The water oxidation half reaction in water splitting for hydrogen production is extremely rate-limiting. This study reports the synthesis of two heterometallic clusters (Gd₆Cu₂₄-IM and Gd₆Cu₂₄-AC) for application as efficient water oxidation catalysts. Interestingly, the maximum turnover frequency of Gd₆Cu₂₄-IM in an NaAc solution of a weak acid (pH 6) was 319 s⁻¹. The trimetallic catalytic site, H₂O–Gd^IIICu^II₂–H₂O, underwent two consecutive two-electron two-proton coupled transfer processes to form high-valent Gd^III–O–O–Cu^III₂ intermediates. Furthermore, the O–O bond was formed via intramolecular interactions between the Cu^III and Gd^III centers. The results of this study revealed that synergistic catalytic water oxidation between polymetallic sites can be an effective strategy for regulating O–O bond formation.

This article is part of the themed collection: 2023 Chemical Science HOT Article Collection

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DOI: https://doi.org/10.1039/D3SC05849B
Article type: Edge Article
Submitted: 02 Nov 2023
Accepted: 04 Dec 2023
First published: 05 Dec 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry

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Chem. Sci., 2024,15, 511-515

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Soluble Gd₆Cu₂₄ clusters: effective molecular electrocatalysts for water oxidation

J. Chen, Z. Pan, Q. Qiu, C. Wang, L. Long, L. Zheng and X. Kong, Chem. Sci., 2024, 15, 511 DOI: 10.1039/D3SC05849B

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