Spin crossover-driven diiron electrocatalyst boosts sustainable water oxidation

Ching-Wei Tung, Wei Zhang (), Tai Ying Lai, Jiali Wang, You-Chiuan Chu, Guan-Bo Wang, Chia-Shuo Hsu, Yen-Fa Liao, Nozomu Hiraoka, Hirofumi Ishii, Xiao Cheng Zeng () and Hao Ming Chen ()
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Ching-Wei Tung: National Taiwan University
Wei Zhang: Jiangsu University
Tai Ying Lai: National Taiwan University
Jiali Wang: National Taiwan University
You-Chiuan Chu: National Taiwan University
Guan-Bo Wang: National Taiwan University
Chia-Shuo Hsu: National Synchrotron Radiation Research Center
Yen-Fa Liao: National Synchrotron Radiation Research Center
Nozomu Hiraoka: National Synchrotron Radiation Research Center
Hirofumi Ishii: National Synchrotron Radiation Research Center
Xiao Cheng Zeng: City University of Hong Kong
Hao Ming Chen: National Taiwan University

Nature Sustainability, 2025, vol. 8, issue 7, 793-805

Abstract: Abstract Electrocatalytic reduction of carbon dioxide and water oxidation are promising technologies to mitigate environmental problems. A critical bottleneck, however, is the significant energy loss that arises from the anodic oxygen evolution reaction (OER) with its sluggish kinetics and reliance on scarce noble metals. It is therefore essential to develop earth-abundant and efficient OER catalysts. Here we report the reactive diiron electrocatalyst [Fe2(µ-O)(µ-OH)(L1)2], where L1 is a nitrogen-based ligand, which exhibits an outstanding performance—achieving a turnover frequency of 20.2 s−1 at 1.580 V and a low overpotential of 184 mV at a current density of 10 mA cm−2—and exceptional stability over 1,000 h. This diiron electrocatalyst is formed via a spin crossover-driven dimerization mechanism, where the resulting diiron atomic configuration promotes strong metal–ligand covalency and facilitates the formation of key intermediates that are essential for efficient OER catalysis. Our findings offer a promising strategy for the design of high-performance catalysts for water oxidation and sustainable electrocatalysis.

Date: 2025
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DOI: 10.1038/s41893-025-01571-3

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