Manipulating the Water Dissociation Electrocatalytic Sites of Bimetallic Nickel‐Based Alloys for Highly Efficient Alkaline Hydrogen Evolution

Transition‐metal alloys are currently drawing increasing attention as promising electrocatalysts for the alkaline hydrogen evolution reaction (HER). However, traditional density‐functional‐theory‐derived d‐band theory fails to describe the hydrogen adsorption energy (ΔGH) on hollow sites. Herein, by...

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Veröffentlicht in:Angewandte Chemie International Edition 2022-07, Vol.61 (30), p.e202202518-n/a
Hauptverfasser: Wang, Jinsong, Xin, Sisi, Xiao, Yao, Zhang, Zhengfu, Li, Zhimin, Zhang, Wang, Li, Caiju, Bao, Rui, Peng, Jian, Yi, Jianhong, Chou, Shulei
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Sprache:eng
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Zusammenfassung:Transition‐metal alloys are currently drawing increasing attention as promising electrocatalysts for the alkaline hydrogen evolution reaction (HER). However, traditional density‐functional‐theory‐derived d‐band theory fails to describe the hydrogen adsorption energy (ΔGH) on hollow sites. Herein, by studying the ΔGH for a series of Ni−M (M=Ti, V, Cr, Mn, Fe, Co, Cu, Zn, Mo, W) bimetallic alloys, an improved d‐band center was provided and a potential NiCu electrocatalyst with a near‐optimal ΔGH was discovered. Moreover, oxygen atoms were introduced into Ni−M (O−NiM) to balance the adsorption/desorption of hydroxyl species. The tailored electrocatalytic sites for water dissociation can synergistically accelerate the multi‐step alkaline HER. The prepared O−NiCu shows the optimum HER activity with a low overpotential of 23 mV at 10 mA cm−2. This work not only broadens the applicability of d‐band theory, but also provides crucial understanding for designing efficient HER electrocatalysts. An improved d‐band model is presented as a valid descriptor to reflect hollow‐site adsorption and hydrogen evolution reaction (HER) activity for multi‐elemental alloy catalysts. NiCu was found to have a near‐optimal ΔGH value and the introduction of O atoms into the Ni−Cu surface could accelerate water dissociation. Tailoring electrocatalytic sites for water dissociation can synergistically complete the multi‐step reactions of alkaline HER.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202202518