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电子在NiWO-NiO活性位点上的重新分布会在碱性介质中协同增强析氢反应。

Electronic redistribution over the active sites of NiWO-NiO induces collegial enhancement in hydrogen evolution reaction in alkaline medium.

作者信息

Gaur Ashish, Pundir Vikas, Maruyama Takahiro, Bera Chandan, Bagchi Vivek

机构信息

Institute of Nano Science and Technology, Sector-81, Knowledge City, Sahibzada Ajit Singh Nagar, Punjab 140306, India.

Department of Applied Chemistry, Meijo University, 1-501 Shiogamaguchi, Tempaku, Nagoya 468-8502, Japan.

出版信息

J Colloid Interface Sci. 2023 Jul;641:82-90. doi: 10.1016/j.jcis.2023.02.153. Epub 2023 Mar 5.

Abstract

The activity-enhancement of a new-generation catalyst focuses on the collegial approach among specific solids which exploit the mutual coactions of these materials for HER applications. Strategic manipulation of these solid interfaces typically reveals unique electronic states different from their pure phases, thus, providing a potential passage to create catalysts with excellent activity and stability. Herein, the formation of the NiWO-NiO interface has been designed and synthesized via a three-step method. This strategy enhances the chance of the formation of abundant heterointerfaces due to the fine distribution of NiWO nanoparticles over Ni(OH) sheets. NiWO-NiO has superior HER activity in an alkaline (1 M KOH) electrolyte with modest overpotentials of 68 mV at 10 mA cm current density. The catalyst is highly stable in an alkaline medium and negligible change was observed in the current density even after 100 h of continuous operation. This study explores a unique method for high-performance hydrogen generation by constructing transition metal-oxides heterojunction. The XPS studies reveal an electronic redistribution driven by charge transfer through the NiWO-NiO interface. The density functional theory (DFT) calculations show that the NiWO-NiO exhibits a Pt-like activity with the hydrogen Gibbs free energy (ΔG*) value of 0.06 eV compared to the Pt(ΔG* = -0.02 eV).

摘要

新一代催化剂的活性增强聚焦于特定固体之间的协同方法,该方法利用这些材料的相互作用来实现析氢反应(HER)应用。对这些固体界面的策略性调控通常会揭示出与其纯相不同的独特电子态,因此,为制备具有优异活性和稳定性的催化剂提供了一条潜在途径。在此,通过三步法设计并合成了NiWO-NiO界面。由于NiWO纳米颗粒在Ni(OH)片上的精细分布,该策略增加了形成大量异质界面的机会。在碱性(1 M KOH)电解液中,NiWO-NiO具有优异的析氢活性,在10 mA cm电流密度下的过电位适中,为68 mV。该催化剂在碱性介质中高度稳定,即使连续运行100小时后,电流密度也观察到可忽略不计的变化。本研究探索了一种通过构建过渡金属氧化物异质结来实现高效制氢的独特方法。X射线光电子能谱(XPS)研究揭示了通过NiWO-NiO界面的电荷转移驱动的电子重新分布。密度泛函理论(DFT)计算表明,NiWO-NiO表现出类似铂的活性,氢吉布斯自由能(ΔG*)值为0.06 eV,而铂的ΔG* = -0.02 eV。

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