Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides.,Angewandte Chemie International Edition

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Atomic Imaging of Subsurface Interstitial Hydrogen and Insights into Surface Reactivity of Palladium Hydrides.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-07-04 , DOI: 10.1002/anie.202006562
Bingqing Lin ₁ , Xi Wu ₁ , Lin Xie ₂ , Yongqiang Kang ₁ , Hongda Du ₁ , Feiyu Kang ₁ , Jia Li ₁ , Lin Gan ₁

Affiliation

Resolving interstitial hydrogen atoms at the surfaces and interfaces is crucial for understanding the mechanical and physicochemical properties of metal hydrides. Although palladium (Pd) hydrides hold important applications in hydrogen storage and electrocatalysis, the atomic position of interstitial hydrogen at Pd hydride near surfaces still remains undetermined. We report the first direct imaging of subsurface hydrogen atoms absorbed in Pd nanoparticles by using differentiated and integrated differential phase contrast within an aberration‐corrected scanning transmission electron microscope. In contrast to the well‐established octahedral interstitial sites for hydrogen in the bulk, subsurface hydrogen atoms are directly identified to occupy the tetrahedral interstices. DFT calculations show that the amount and the occupation type of subsurface hydrogen atoms play an indispensable role in fine‐tuning the electronic structure and associated chemical reactivity of the Pd surface.

中文翻译：

地下间隙氢的原子成像和对钯氢化物表面反应性的认识。

解决表面和界面上的间隙氢原子对于理解金属氢化物的机械和物理化学特性至关重要。尽管氢化钯（Pd）在储氢和电催化方面具有重要的应用，但在表面附近的氢化钯上的间隙氢原子位置仍未确定。我们通过在像差校正的扫描透射电子显微镜内使用微分和积分微分相衬报告了Pd纳米颗粒中吸收的地下氢原子的首次直接成像。与在体积中为氢确定的八面体间隙位置相反，地下氢原子被直接识别为占据四面体间隙。

更新日期：2020-07-04

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