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强碱性条件下镍基掺杂单原子铂的析氢反应

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

作者信息

An Xiurui, Yao Ting-Ting, Liu Yang, Long Guifa, Wang Aoqi, Feng Zhendong, Dupuis Michel, Li Can

机构信息

State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China.

Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, 100049 Beijing, China.

出版信息

J Phys Chem Lett. 2023 Sep 14;14(36):8121-8128. doi: 10.1021/acs.jpclett.3c02142. Epub 2023 Sep 5.

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 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 H 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 H formation from surface H on Ni-Pt(SAs).

摘要

铂催化剂被认为是酸性条件下析氢反应(HER)的最先进催化剂。然而,其在碱性条件下的催化动力学尚未得到充分理解。在此,我们报道了一种镍-铂单原子(SAs)催化剂,其中铂原子分散在镍基体中,在强碱性电解质(7 M KOH)中,在500 mA cm时,其析氢性能令人印象深刻,过电位低至210 mV,远高于铂纳米颗粒修饰的镍催化剂(Ni-Pt(NPs))。动力学分析表明,镍基体中的铂掺杂可以加速镍-铂表面的沃尔默步骤。此外,在高电流密度下,Ni-Pt(SAs)比Ni-Pt(NPs)表现出更有利于氢形成反应的动力学。理论计算表明,原子分散的铂减弱了镍-铂电极表面氢和羟基的吸附,并促进了Ni-Pt(SAs)表面氢形成氢。

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