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钌纳米颗粒上铂原子的排列如何提高析氢活性。

How the Arrangement of Platinum Atoms on Ruthenium Nanoparticles Improves Hydrogen Evolution Activity.

作者信息

Li Qinyu, Cheong Soshan, Poerwoprajitno Agus R, Xiang Shuting, Frenkel Anatoly I, Yang Yuwei, Bedford Nicholas M, Umer Sohaib, Lessio Martina, Ohnishi Ichiro, Ramadhan Zeno R, Huber Dale L, Dai Liming, Schuhmann Wolfgang, Gooding J Justin, Tilley Richard D

机构信息

School of Chemistry, University of New South Wales, Sydney, NSW, 2052, Australia.

Mark Wainwright Analytical Centre, University of New South Wales, Sydney, NSW, 2052, Australia.

出版信息

Adv Mater. 2025 Jul 22:e09610. doi: 10.1002/adma.202509610.

DOI:10.1002/adma.202509610
PMID:40693347
Abstract

The platinum-ruthenium (PtRu) system is highly active for hydrogen evolution reaction (HER) in alkaline media with both Pt and Ru playing active roles in the water dissociation step that generates adsorbed hydrogen atoms. Precise control of the arrangement of Pt atoms on Ru nanoparticles can maximize the Pt-Ru sites for water dissociation and Pt-Pt sites for hydrogen production and can considerably improve HER catalytic performance. By directing the growth and distribution of Pt on Ru hourglass nanoparticles, the arrangement of Pt on Ru is controlled into forming Pt islands, small Pt clusters, and strings of a few Pt atoms. Calculations show that the unique atomic string arrangements of Pt on Ru is the thermodynamically favorable configuration. Additionally, these strings have a favorable combination of Pt-Ru and Pt-Pt sites, making the Pt-string on Ru the most active catalyst with a more than fivefold increase in turnover frequency for alkaline HER compared to the Pt-island on Ru catalyst. The results show how controlling the Pt atomic arrangement on Ru nanoparticle surfaces for the tuning of Pt-Pt and Pt-Ru neighboring sites can direct toward a more efficient HER mechanism and thereby significantly enhancing HER performance.

摘要

铂钌(PtRu)体系在碱性介质中对析氢反应(HER)具有高活性,其中Pt和Ru在生成吸附氢原子的水离解步骤中均发挥着活性作用。精确控制Ru纳米颗粒上Pt原子的排列,可以使水离解的Pt-Ru位点和产氢的Pt-Pt位点最大化,并能显著提高HER催化性能。通过引导Pt在Ru沙漏形纳米颗粒上的生长和分布,将Pt在Ru上的排列控制为形成Pt岛、小Pt簇和由几个Pt原子组成的链。计算表明,Pt在Ru上独特的原子链排列是热力学上有利的构型。此外,这些链具有有利的Pt-Ru和Pt-Pt位点组合,使得Ru上的Pt链成为最活跃的催化剂,与Ru上的Pt岛催化剂相比,碱性HER的周转频率增加了五倍以上。结果表明,通过控制Ru纳米颗粒表面的Pt原子排列来调节Pt-Pt和Pt-Ru相邻位点,可导向更高效的HER机制,从而显著提高HER性能。

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