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

Angewandte Chemie Pub Date : 2022-04-19 DOI:10.1002/ange.202202518

Dr. Jinsong Wang, Sisi Xin, Prof. Yao Xiao, Prof. Zhengfu Zhang, Zhimin Li, Dr. Wang Zhang, Prof. Caiju Li, Prof. Rui Bao, Dr. Jian Peng, Prof. Jianhong Yi, Prof. Shulei Chou

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引用次数: 1

Abstract

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 (ΔG_H) on hollow sites. Herein, by studying the ΔG_H 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 ΔG_H 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.

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操纵双金属镍基合金水解离电催化位点的高效碱性析氢

过渡金属合金作为碱析氢反应的电催化剂，近年来受到越来越多的关注。然而，传统的密度泛函理论衍生的d波段理论无法描述氢在空心位点上的吸附能(ΔGH)。本文通过研究一系列Ni−M (M=Ti, V, Cr, Mn, Fe, Co, Cu, Zn, Mo, W)双金属合金的ΔGH，提供了一个改进的d波段中心，并发现了一个具有接近最优ΔGH的潜在NiCu电催化剂。此外，在Ni−M (O−NiM)中引入氧原子来平衡羟基的吸附/解吸。定制的水解离电催化位点可协同加速多步碱性HER反应。制备的O−NiCu在10 mA cm−2下的过电位为23 mV，具有最佳的HER活性。这项工作不仅拓宽了d波段理论的适用性，而且为设计高效的HER电催化剂提供了重要的理解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Angewandte Chemie 化学科学, 有机化学, 有机合成

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0.00%

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审稿时长

1 months