Yu Jun, Gu Xinyu, Sun Huiyu, Zhang Nannan, Hata Shinichi, Liu Tianpeng, Wu Zhengying, Shiraishi Yukihide, Du Yukou
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Industrial Park, Renai Road, Suzhou 215123, PR China.
Department of Applied Chemistry, Faculty of Engineering, Sanyo-Onoda City University, Sanyo Onoda, Yamaguchi 756-0884, Japan.
J Colloid Interface Sci. 2025 Dec 15;700(Pt 1):138429. doi: 10.1016/j.jcis.2025.138429. Epub 2025 Jul 12.
The design of high-quality bifunctional catalyst is the hinge to promoting the development of hydrogen production technology. Doping engineering has been validated as an effective modification strategy for optimizing the intrinsic activity of the catalyst. Herein, a FeNiS@Cr-NiFe LDH heterostructure electrocatalyst with an enhanced built-in electric field (BIEF) and activated lattice oxygen is reported. Cr doping significantly reduces the activation barrier of lattice oxygen and promotes the dynamic reconstruction of the oxygen coordination environment. This process drives the transformation of the oxygen evolution reaction (OER) mechanism into a kinetically favorable lattice oxygen mechanism (LOM), which allows the catalyst to exhibit outstanding OER performance. Additionally, the enhanced BIEF improves the driving force for the directional movement of electrons, accelerating the supply of electrons in the Volmer step of the hydrogen evolution reaction (HER) mechanism, thereby optimizing the HER activity of the material. Accordingly, the FeNiS@Cr-NiFe LDH electrocatalyst displays outstanding OER (η = 217 mV, η = 232 mV) and HER (η = 162 mV, η = 222 mV) performance, as well as superior catalytic stability. This study focuses on the regulation of BIEF and activation of lattice oxygen, which offers a fresh perspective into the design of bifunctional catalysts based on BIEF and LOM.
高质量双功能催化剂的设计是推动制氢技术发展的关键。掺杂工程已被证实是一种优化催化剂本征活性的有效改性策略。在此，报道了一种具有增强内建电场（BIEF）和活化晶格氧的FeNiS@Cr-NiFe LDH异质结构电催化剂。Cr掺杂显著降低了晶格氧的活化能垒，并促进了氧配位环境的动态重构。这一过程推动析氧反应（OER）机制转变为动力学有利的晶格氧机制（LOM），使催化剂表现出优异的OER性能。此外，增强的BIEF提高了电子定向移动的驱动力，加速了析氢反应（HER）机制中Volmer步骤的电子供应，从而优化了材料的HER活性。因此，FeNiS@Cr-NiFe LDH电催化剂表现出优异的OER（η = 217 mV，η = 232 mV）和HER（η = 162 mV，η = 222 mV）性能以及卓越的催化稳定性。本研究聚焦于BIEF的调控和晶格氧的活化，为基于BIEF和LOM的双功能催化剂设计提供了新的视角。
