Engineering all-organic electrocatalysts with asymmetric dual-active sites for uncommon oxygen-evolving pathway.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 42414322.
- Also identified by DOI 10.1038/s41467-026-75304-1.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
The performance of electrocatalytic oxygen evolution reaction is governed by molecular evolution pathways, yet their regulation remains a significant experimental and theoretical hurdle. Herein, we propose the construction of asymmetric non-metallic dual-active sites through engineering hydroxyl groups in an all-organic electrocatalyst, thereby triggering an uncommon asymmetric oxide pathway mechanism. This reaction pathway reduces the requirement of strict equilibrium on adsorption energies at dual-active sites for traditional oxide pathway mechanism, and also avoids the limitation of the linear scaling relationship for adsorbate evolution mechanism. Therefore, the proposed metal-free electrocatalyst shows competitive oxygen evolution reaction performance with an overpotential of 364.3 ± 4.5 mV at 1.0 A·cm<sup>-2</sup>. Combining operando spectroscopic/mass spectrometry and theoretical calculations unveils that the asymmetric oxide pathway mechanism undergoes the critical step of *OH intramolecular nucleophilic attack to neighboring *O, forming *OOH with drastically reducing energy barriers. This work shows the diversity of oxygen evolution pathways in all-organic electrocatalysts and offers a viewpoint for optimizing the electrocatalytic performances of metal-free solids.