High-spin transition metal atoms drive acidic oxygen evolution reactions.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41708642.
- Also identified by DOI 10.1038/s41467-026-69682-9 and PMC identifier 13031339.
- Licence recorded as CC BY-NC-ND.
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Abstract
Synthesizing transition metal catalysts to replace precious metal ones such as IrO<sub>2</sub> and RuO<sub>2,</sub> achieving efficient acidic oxygen evolution reaction while balancing intrinsic activity, stability, and cost-effectiveness always been a dream pursued by scientists and industrialists, but still remains a challenge. Here, we present an efficient catalytic system formed by graphdiyne-induced high-spin state cobalt-based oxide (HSS-CoO<sub>x</sub>/GDY) for enhancing the activity and stability of the acidic oxygen evolution reaction. Experimental and theoretical results demonstrate that the bonding of electron-rich sp-hybridized carbon and Co atoms initiates the Jahn-Teller effect of CoO<sub>6</sub> octahedra, which regulates the occupied d-orbital of Co atoms and generates the high-spin Co<sup>3+</sup>. Such spin occupancy breaks the spin-forbidden effect and optimizes the adsorption/desorption ability of HSS-CoO<sub>x</sub>/GDY toward key reaction intermediates, thereby promoting the coupling of O-O bonds and the evolution of oxygen gas. The proton exchange membrane water electrolyzers constructed based on this catalyst achieve a current density of 1.0 A cm<sup>-2</sup> at a low cell voltage of 1.80 V. This research indicates that graphdiyne has the ability to manipulate the electronic spin states of electrocatalysts.