Atomic-scale self-rearrangement of hetero-metastable phases into high-density single-atom catalysts for the oxygen evolution reaction.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 40133310.
- Also identified by DOI 10.1038/s41467-025-58163-0 and PMC identifier 11937230.
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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-Ir<sub>SA</sub>) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH)<sub>2</sub> substrates. The CoCe-O-Ir<sub>SA</sub> delivers an overpotential of 187 mV at 100 mA cm<sup>-2</sup> and a steady lifespan of 1000 h at 500 mA cm<sup>-2</sup> for oxygen evolution reaction. Furthermore, the CoCe-O-Ir<sub>SA</sub> is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm<sup>-2</sup> 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.