Updating the sub-nanometric cognition of reconstructed oxyhydroxide active phase for water oxidation.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 40159508.
- Also identified by DOI 10.1038/s41467-025-58424-y and PMC identifier 11955520.
- Licence recorded as CC BY-NC-ND.
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Abstract
Unveiling structure-activity correlations at the sub-nanoscale remains an essential challenge in catalysis science. During electrocatalysis, dynamic structural evolution drives the ambiguous entanglement of crystals and electrons degrees of freedom that obscure the activity origin. Here, we track the structural evolution of Ni-based model pre-catalysts (Ni(OH)<sub>2</sub>, NiS<sub>2</sub>, NiSe<sub>2</sub>, NiTe), detailing their catalytically active state during water oxidation via operando techniques and theoretical calculations. We reveal the sub-nanometric structural difference of NiO<sub>6</sub> unit with a regular distortion in the reconstructed active phase NiOOH, codetermined by the geometric (bond lengths) and electronic (covalency) structure of the pre-catalysts on both spatial and temporal scales. The symmetry-broken active units induce the delicate balance of the p and d orbitals in NiOOH, further steering the modulation of catalytic intermediate configurations and mechanisms, with improved performance. This work recognizes the fine structural differences of the active phases from the sub-nanometer scale, and quantitatively explains their influence on activity. Our findings provide a more intuitive design framework for high-efficiency materials through targeted symmetry engineering of active units.