Deciphering the role of ultra-low-loaded rhodium in NiFe-MIL-53 for superior oxygen evolution reaction

被引：3

作者：

Jia, Jinzhi ^{[1
]}

Zhang, Jinhua ^{[1
]}

Guo, Kailu ^{[2
]}

Zhang, Lanyue ^{[1
]}

Du, Gening ^{[1
]}

You, Hao ^{[1
]}

Huang, Junfeng ^{[1
]}

Tu, Mudong ^{[1
]}

Li, Hua ^{[1
]}

Peng, Yong ^{[1
]}

Dou, Wei ^{[1
]}

Xu, Cailing ^{[1
]}

机构：

[1] Lanzhou Univ, Coll Chem & Chem Engn, Sch Mat & Energy, State Key Lab Appl Organ Chem, Lanzhou 730000, Gansu, Peoples R China

[2] LuoYang Normal Univ, Coll Chem & Chem Engn, Luoyang 471934, Henan, Peoples R China

来源：

JOURNAL OF ENERGY CHEMISTRY | 2025年 / 100卷

关键词：

NiFe-MIL-53; Rh; Electrochemical reconstruction; Catalytic mechanism; Oxygen evolution reaction; METAL-ORGANIC-FRAMEWORK; RECONSTRUCTION;

D O I：

10.1016/j.jechem.2024.08.022

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

Designing highly active and stable electrocatalysts of oxygen evolution reaction (OER) is one of the crucial challenges. In this study, a novel OER electrocatalyst, NiFe-MIL-53 modified with ultra-low rhodium (Rh@NiFe-MIL-53), is successfully prepared via the hydrothermal method. In-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active species. More importantly, the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe(OH)2 after doping Rh is beneficial for improving the electrochemical stability of the catalyst. X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@NiFeOOH. Furthermore, theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap, regulates the d-band center (ed), accelerates the charge transfer, and optimizes the adsorption behavior of oxygen-containing intermediates, thereby lowering the energy barrier of rate-determining steps. Consequently, the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity (240 mV) with a small Tafel slope of 48.2 mV dec-1 and long-term durability (over 1270 h at 10 mA cm-2 and 110 hat 200 mA cm-2). This work presents a new perspective on designing highly efficient OER electrocatalysts. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

引用

页码：77 / 86

页数：10