Overlayer Stacking Promotes Hydrogen Spillover

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-09-29 DOI:10.1021/acs.nanolett.5c04009

Jinqiu Guo, Hongbo Zhang

引用次数: 0

Abstract

Hydrogen spillover (HSO) has attracted significant attention due to its important role in elucidating the synergistic interactions between separated active sites during catalysis; however, it is controversial since the driving force of hydrogen migration is unclear. Herein, atomic layer deposition (ALD) was employed to spatially separate well-defined Pd/Ni nanoparticles (NPs), enabling the clear identification of HSO at mild reaction conditions (i.e., 343 K) during alkyne semihydrogenation over aNi/nMO_x/Pd@support catalysts, in which Pd is unreachable. Interestingly, ALD stacking of the Ti-, Zr-, Zn-, or Al-oxide overlayers significantly enhanced the HSO, attributed to the “chimney effect”, and the driving force of hydrogen migration was attributed to the concentration difference between Pd-NPs and Ni-NPs during catalysis.

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叠加层促进氢溢出

氢溢出效应（HSO）在阐明分离活性位点在催化过程中的协同作用方面起着重要作用，引起了人们的广泛关注。然而，由于氢迁移的驱动力尚不清楚，因此存在争议。本文采用原子层沉积（ALD）技术在空间上分离定义良好的Pd/Ni纳米颗粒（NPs），从而在aNi/nMOx/Pd@support催化剂上进行的炔半加氢反应中，在温和的反应条件（即343 K）下，能够清晰地识别HSO，而在这种条件下，Pd是无法获得的。有趣的是，Ti-、Zr-、Zn-或al -氧化物覆盖层的ALD叠加显著增强了HSO，这归因于“烟囱效应”，氢迁移的驱动力归因于催化过程中Pd-NPs和Ni-NPs之间的浓度差异。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

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