Affiliation:
1. The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science and Technology Wuhan 430081 P. R. China
2. Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Science Beijing 100190 P. R. China
Abstract
AbstractRecently, conductive metal–organic frameworks (c‐MOFs) have drawn tremendous attention for the application in oxygen evolution reaction (OER) due to their superior conductivity and highly accessible active sites. Herein, a facile method is reported to prepare a series of bimetallic c‐MOFs (NixFe1‐x‐THQ, THQ = tetrahydroxy‐1,4‐benzoquinone hydrate) by using the smallest benzene‐based ligand with high‐density catalytic active sites for OER. By adjusting the ratio of Ni/Fe, a series of catalysts with optimal electronic structures and adsorption capacity to intermediates, and faster charge transport are obtained. Among them, Ni0.5Fe0.5‐THQ exhibits superior catalytic performances for OER with a low overpotential of 272 mV at 10 mA cm−2, a small Tafel slope of 47.9 mV, and robust operation for 40 h with no detectable activity decay, which is far superior to commercial RuO2, most of traditional MOFs and even some monometallic conductive MOFs. Moreover, both the measured and simulated results manifest that Ni0.5Fe0.5‐THQ can tailor the d‐band center, and induce the directional transfer of electrons, optimizing the rate‐determining step and adsorption capacity to intermediates during OER, thus exhibits superior electrochemical activity. This work not only presents a strategy to fabricate an electrocatalyst with remarkable OER performance but also promotes the development of THQ‐based c‐MOFs for electrocatalysis.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Hubei Province
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials