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Electronic Modulation Caused by Interfacial Ni‐O‐M (M=Ru, Ir, Pd) Bonding for Accelerating Hydrogen Evolution Kinetics
Author(s) -
Deng Liming,
Hu Feng,
Ma Mingyue,
Huang ShaoChu,
Xiong Yixing,
Chen HanYi,
Li Linlin,
Peng Shengjie
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202110374
Subject(s) - catalysis , redistribution (election) , adsorption , noble metal , kinetics , metal , nickel , nanoparticle , hydrogen bond , chemistry , hydrogen , redox , electron transfer , materials science , chemical engineering , chemical physics , inorganic chemistry , nanotechnology , molecule , organic chemistry , physics , engineering , quantum mechanics , politics , political science , law
Designing definite metal‐support interfacial bond is an effective strategy for optimizing the intrinsic activity of noble metals, but rather challenging. Herein, a series of quantum‐sized metal nanoparticles (NPs) anchored on nickel metal–organic framework nanohybrids (M@Ni‐MOF, M=Ru, Ir, Pd) are rationally developed through a spontaneous redox strategy. The metal‐oxygen bonds between the NPs and Ni‐MOF guarantee structural stability and sufficient exposure of the surface active sites. More importantly, such precise interfacial feature can effectively modulate the electronic structure of hybrids through the charge transfer of the formed Ni‐O‐M bridge and then improves the reaction kinetics. As a result, the representative Ru@Ni‐MOF exhibits excellent hydrogen evolution reaction (HER) activity at all pH values, even superior to commercial Pt/C and recent noble‐metal catalysts. Theoretical calculations deepen the mechanism understanding of the superior HER performance of Ru@Ni‐MOF through the optimized adsorption free energies of water and hydrogen due to the interfacial‐bond‐induced electron redistribution.