Dual-site segmentally synergistic catalysis mechanism: boosting CoFeS<sub>x</sub> nanocluster for sustainable water oxidation.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38409270.
- Also identified by DOI 10.1038/s41467-024-45700-6 and PMC identifier 10897303.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Efficient oxygen evolution reaction electrocatalysts are essential for sustainable clean energy conversion. However, catalytic materials followed the conventional adsorbate evolution mechanism (AEM) with the inherent scaling relationship between key oxygen intermediates *OOH and *OH, or the lattice-oxygen-mediated mechanism (LOM) with the possible lattice oxygen migration and structural reconstruction, which are not favorable to the balance between high activity and stability. Herein, we propose an unconventional Co-Fe dual-site segmentally synergistic mechanism (DSSM) for single-domain ferromagnetic catalyst CoFeS<sub>x</sub> nanoclusters on carbon nanotubes (CNT) (CFS-ACs/CNT), which can effectively break the scaling relationship without sacrificing stability. Co<sup>3+</sup> (L.S, t<sub>2g</sub><sup>6</sup>e<sub>g</sub><sup>0</sup>) supplies the strongest OH* adsorption energy, while Fe<sup>3+</sup> (M.S, t<sub>2g</sub><sup>4</sup>e<sub>g</sub><sup>1</sup>) exposes strong O* adsorption. These dual-sites synergistically produce of Co-O-O-Fe intermediates, thereby accelerating the release of triplet-state oxygen ( ↑ O = O ↑ ). As predicted, the prepared CFS-ACs/CNT catalyst exhibits less overpotential than that of commercial IrO<sub>2</sub>, as well as approximately 633 h of stability without significant potential loss.