Ir Single Atoms Boost Metal–Oxygen Covalency on Selenide-Derived NiOOH for Direct Intramolecular Oxygen Coupling
- Type: Journal Article
- Author: Yin, Zhao-Hua; Huang, Yuan; Song, Kepeng; Li, Tian-Tian; Cui, Jun-Yuan; Meng, Chao; Zhang, Huigang; Wang, Jian-Jun
- Journal: Journal of the American Chemical Society
- Volume: Not supported.
- Issue: Not supported.
- Pages: Not supported.
- Year: 2024
- DOI: 10.1021/jacs.3c13746
Abstract
This investigation probes the intricate interplay of catalyst dynamics and reaction pathways during the oxygen evolution reaction (OER), highlighting the significance of atomic-level and local ligand structure insights in crafting highly active electrocatalysts. Leveraging a tailored ion exchange reaction followed by electrochemical dynamic reconstruction, we engineered a novel catalytic structure featuring single Ir atoms anchored to NiOOH (Ir1@NiOOH). This novel approach involved the strategic replacement of Fe with Ir, facilitating the transition of selenide precatalysts into active (oxy)hydroxides. This elemental substitution promoted an upward shift in the O 2p band and intensified the metal–oxygen covalency, thereby altering the OER mechanism toward enhanced activity. The shift from a single-metal site mechanism (SMSM) in NiOOH to a dual-metal-site mechanism (DMSM) in Ir1@NiOOH was substantiated by in situ differential electrochemical mass spectrometry (DEMS) and supported by theoretical insights. Remarkably, the Ir1@NiOOH electrode exhibited exceptional electrocatalytic performance, achieving overpotentials as low as 142 and 308 mV at current densities of 10 and 1000 mA cm–2, respectively, setting a new benchmark for the electrocatalysis of OER.
Files and Links
- Url: https://doi.org/10.1021/jacs.3c13746
- Local Library: Zotero