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Enhanced Metallicity Boosts Hydrogen Evolution Capability of Dual-Bimetallic Ni-Fe Nitride Nanoparticles
Materials Today Physics ( IF 11.5 ) Pub Date : 2020-12-01 , DOI: 10.1016/j.mtphys.2020.100267
Yuwen Hu , Tuzhi Xiong , M.-Sadeeq Jie Tang Balogun , Yongchao Huang , David Adekoya , Shanqing Zhang , Yexiang Tong

Abstract Enriching electrocatalysts with uncommon definite functions are of great influence but remains extraordinarily challenging. Upon the excellent metallic characteristics of transition metal nitrides (TMN), the unfavorable d-band energy level severely hinders their hydrogen evolution reaction (HER) catalytic properties. Herein, a new concept termed “enhanced metallicity” is introduced to address this issue. We strongly enable bimetallic Ni2Fe2N with outstanding alkaline HER capability by making more metallic through in situ hybridization of another bimetallic compound, Ni3Fe. The enhanced metallicity Ni2Fe2N/Ni3Fe hybrid displays nearly 200% enhancement in alkaline HER catalytic activity compared to pristine Ni2Fe2N at a current density of 10 mA cm-2. Experimental and theoretical analyses, as well as crystal field diagram persistently show that the enhanced HER catalytic properties is attributed to the enhanced metallic nature and synergistic effect, endowing strong electronic interaction between Ni2Fe2N and Ni3Fe. The strong electronic interaction enables low adsorption energy and a reasonable shift in the d-orbital, which helps in facilitating water dissociation and H-desorption. This present study offers a useful pathway for the rational design of other catalysts for HER and beyond.

中文翻译:

增强的金属性提高了双双金属 Ni-Fe 氮化物纳米颗粒的析氢能力

摘要 富集具有特殊功能的电催化剂具有很大的影响,但仍然极具挑战性。由于过渡金属氮化物 (TMN) 具有优异的金属特性,不利的 d 带能级严重阻碍了它们的析氢反应 (HER) 催化性能。在此,引入了一个称为“增强金属度”的新概念来解决这个问题。我们通过另一种双金属化合物 Ni3Fe 的原位杂化来制造更多金属,从而使双金属 Ni2Fe2N 具有出色的碱性 HER 能力。在 10 mA cm-2 的电流密度下,与原始 Ni2Fe2N 相比,增强的金属性 Ni2Fe2N/Ni3Fe 混合体在碱性 HER 催化活性方面显示出近 200% 的增强。实验和理论分析,以及晶体场图持续表明,增强的 HER 催化性能归因于增强的金属性质和协同效应,赋予 Ni2Fe2N 和 Ni3Fe 之间强的电子相互作用。强大的电子相互作用使低吸附能和 d 轨道的合理转移,有助于促进水解离和 H 解吸。本研究为合理设计其他用于 HER 及其他催化剂的催化剂提供了有用的途径。
更新日期:2020-12-01
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