Wu Zhi-Peng, Zuo Shouwei, Pei Zhihao, Zhang Jing, Zheng Lirong, Luan Deyan, Zhang Huabin, Lou Xiong Wen David
School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore.
KAUST Catalysis Center (KCC), Division of Physical Science and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900, Saudi Arabia.
Sci Adv. 2025 Mar 7;11(10):eadu5370. doi: 10.1126/sciadv.adu5370.
Non-noble metal-based heteroatom compounds demonstrate excellent electrocatalytic activity for the oxygen evolution reaction (OER). However, the origin of this activity, driven by structure evolution effects, remains unclear due to the lack of effective in situ/operando techniques. Herein, we employ the operando quick-scan x-ray absorption fine structure (Q-XAFS) technique coupled with in situ controlled electrochemical potential to establish a structure-activity correlation of the OER catalyst. Using Ni-Fe bimetallic phosphides as a model catalyst, operando Q-XAFS experiments reveal that the structural transformation initiates at the preferential oxidation of Fe sites over Ni sites. The in situ-generated O-Fe-P structure serves as the origin of the enhanced electrocatalytic OER activity of the catalyst, a finding supported by theoretical calculations. This work provides crucial insights into understanding the reaction mechanism of the state-of-the-art Ni-Fe-based OER electrocatalysts, thus advancing the rational design of more efficient OER electrocatalysts.
基于非贵金属的杂原子化合物对析氧反应（OER）表现出优异的电催化活性。然而，由于缺乏有效的原位/ operando技术，由结构演变效应驱动的这种活性的起源仍不清楚。在此，我们采用operando快速扫描X射线吸收精细结构（Q-XAFS）技术结合原位控制电化学电位来建立OER催化剂的结构-活性相关性。使用Ni-Fe双金属磷化物作为模型催化剂，operando Q-XAFS实验表明，结构转变始于Fe位点比Ni位点的优先氧化。原位生成的O-Fe-P结构是催化剂电催化OER活性增强的起源，这一发现得到了理论计算的支持。这项工作为理解最先进的Ni-Fe基OER电催化剂的反应机理提供了关键见解，从而推动了更高效OER电催化剂的合理设计。
