Hydrogen Evolution Reaction on Single-Atom Pt Doped in Ni Matrix under Strong Alkaline Condition

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2023-09-05 DOI:10.1021/acs.jpclett.3c02142
Xiurui An, Ting-ting Yao, Yang Liu, Guifa Long, Aoqi Wang, Zhendong Feng, Michel Dupuis and Can Li*, 
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Abstract

Pt catalyst has been considered as the state-of-the-art catalyst for hydrogen evolution reaction (HER) under acid condition. However, its catalytic kinetics under alkaline conditions is not well-understood. Herein, we report a Ni–Pt(SAs) (SAs = single atoms) catalyst with Pt atomically dispersed in a Ni matrix, and it possesses an impressive HER performance with an overpotential as low as 210 mV at 500 mA cm–2 in strong alkaline electrolyte (7 M KOH), which is much higher than Pt nanoparticle-modified Ni catalyst (Ni–Pt(NPs)). Kinetics analysis reveals that Pt doping in the Ni matrix can accelerate the Volmer step on the Ni–Pt surface. Moreover, Ni–Pt(SAs) displays a more favorable kinetics for H2 formation reaction at high current density than Ni–Pt(NPs). Theoretical calculations reveal that atomically dispersed Pt weakens the adsorption of both H and OH on the surface of Ni–Pt electrode and promotes H2 formation from surface H on Ni–Pt(SAs).

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强碱性条件下单原子Pt掺杂Ni基体的析氢反应
铂催化剂被认为是酸性条件下析氢反应的最先进催化剂。但其在碱性条件下的催化动力学尚不清楚。本文报道了一种将Pt原子分散在Ni基体上的Ni - Pt(SAs) (SAs =单原子)催化剂,在强碱性电解质(7 M KOH)中,其过电位在500 mA cm-2时低至210 mV,远高于Pt纳米粒子修饰的Ni催化剂(Ni - Pt(NPs))。动力学分析表明,在Ni基体中掺杂Pt可以加速Ni - Pt表面的Volmer步进。此外,Ni-Pt (SAs)在高电流密度下比Ni-Pt (NPs)表现出更有利的H2生成动力学。理论计算表明,原子分散的Pt削弱了H和OH在Ni-Pt电极表面的吸附,促进了H表面在Ni-Pt (SAs)上生成H2。
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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