Revealing the role of a bridging oxygen in a carbon shell coated Ni interface for enhanced alkaline hydrogen oxidation reaction
CHEMICAL SCIENCE(2024)
Abstract
Encapsulating metal nanoparticles inside carbon layers is a promising approach to simultaneously improving the activity and stability of electrocatalysts. The role of carbon layer shells, however, is not fully understood. Herein, we report a study of boron doped carbon layers coated on nickel nanoparticles (Ni@BC), which were used as a model catalyst to understand the role of a bridging oxygen in a carbon shell coated Ni interface for the improvement of the hydrogen oxidation reaction (HOR) activity using an alkaline electrolyte. Combining experimental results and density functional theory (DFT) calculations, we find that the electronic structure of Ni can be precisely tailored by Ni-O-C and Ni-O-B coordinated environments, leading to a volcano type correlation between the binding ability of the OH* adsorbate and HOR activity. The obtained Ni@BC with a optimized d-band center displays a remarkable HOR performance with a mass activity of 34.91 mA mgNi-1, as well as superior stability and CO tolerance. The findings reported in this work not only highlight the role of the OH* binding strength in alkaline HOR but also provide guidelines for the rational design of advanced carbon layers used to coat metal electrocatalysts. Boron doped carbon coated nickel shows a remarkable activity in alkaline hydrogen oxidation. Theoretical and experimental results reveal that the Ni-O-C(B) interface in the catalyst can optimize the OHBE of Ni and enhance its HOR performance.
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