Atomic-scale self-rearrangement of hetero-metastable phases into high-density single-atom catalysts for the oxygen evolution reaction

Quan Quan, Yuxuan Zhang, Haifan Li, Wei Wang, Pengshan Xie, Dong Chen, Weijun Wang, You Meng, Di Yin, Yezhan Li, Dongyuan Song, Lijie Chen, Shaohai Li (), Cheng Yang, Takeshi Yanagida, Chun-Yuen Wong, SenPo Yip () and Johnny C. Ho ()
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Quan Quan: City University of Hong Kong
Yuxuan Zhang: City University of Hong Kong
Haifan Li: City University of Hong Kong
Wei Wang: City University of Hong Kong
Pengshan Xie: City University of Hong Kong
Dong Chen: City University of Hong Kong
Weijun Wang: City University of Hong Kong
You Meng: City University of Hong Kong
Di Yin: City University of Hong Kong
Yezhan Li: City University of Hong Kong
Dongyuan Song: Kyushu University
Lijie Chen: China International Marine Containers Offshore Co., Ltd
Shaohai Li: Tsinghua University
Cheng Yang: Tsinghua University
Takeshi Yanagida: Kyushu University
Chun-Yuen Wong: City University of Hong Kong
SenPo Yip: Kyushu University
Johnny C. Ho: City University of Hong Kong

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Maximizing metal-substrate interactions by self-reconstruction of coadjutant metastable phases can be a delicate strategy to obtain robust and efficient high-density single-atom catalysts. Here, we prepare high-density iridium atoms embedded ultrathin CoCeOOH nanosheets (CoCe-O-IrSA) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH)2 substrates. The CoCe-O-IrSA delivers an overpotential of 187 mV at 100 mA cm−2 and a steady lifespan of 1000 h at 500 mA cm−2 for oxygen evolution reaction. Furthermore, the CoCe-O-IrSA is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm−2 for 150 h. Operando experimental and theoretical calculation results demonstrate that the reconstructed thermodynamically stable iridium single atoms act as highly active sites by regulating charge redistribution with strongly p-d-f orbital couplings, enabling electron transfer facilitated, the adsorption energies of intermediates optimized, and the surface reactivity of Co/Ce sites activated, leading to high oxygen evolution performance. These results open up an approach for engineering metastable phases to realize stable single-atom systems under ambient conditions toward efficient energy-conversion applications.

Date: 2025
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DOI: 10.1038/s41467-025-58163-0

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