Unveiling the Activity Origin of M–N–C Supported Nanoparticles for Efficient Electrocatalytic Water Oxidation

作者：Weidong Liang, Yong Zhang, Dongniu Wang, Jianzhao Peng, Jinshuo Zou, Haizhou Li, Zhongxin Song, Manlin Tan, Jun Yu, Lei Zhang · 发表于：The Journal of Physical Chemistry Letters · 年份：2025 · DOI：10.1021/acs.jpclett.5c02852 · 被引用次数：4 · 研究领域：Electrocatalysts for Energy Conversion、Advanced oxidation water treatment、Ammonia Synthesis and Nitrogen Reduction

Optimizing the electronic structures of metal sites is desirable for high intrinsic activity. Incorporated metal atoms in a carbon substrate can establish strong electronic interaction with loaded metal oxides. However, this structure may be unstable in a harsh oxygen evolution reaction (OER) environment. Herein, we take the Ni SA Fe sample of Ni–N–C supported Fe 2 O 3 nanoparticles (NPs) as an example. Both in situ and ex situ characterizations show that the OER activation process facilitates the transformation of Ni single atoms into atomically dispersed NiOOH active species while retaining Fe 2 O 3 NPs. Accordingly, abundant structural defects are formed in the carbon support, enhancing electron transfer and upshifting the d-band center of the NiFe catalyst. As a result, the catalyst exhibits accelerated OER kinetics and optimized adsorption energies for reaction intermediates, delivering outstanding intrinsic activity. A low overpotential of 230 mV at 10 mA cm –2 and a turnover frequency (TOF) more than 9 times higher than that of commercial RuO 2 are achieved.