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Directional Gateway to Metal Oxidation: 3D Chemical Mapping Unfolds Oxygen Diffusional Pathways in Rhodium Nanoparticles
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-04-02 , DOI: 10.1021/acs.jpclett.0c00321
Sten V. Lambeets 1, 2 , Thierry Visart de Bocarmé 2 , Daniel E. Perea 1 , Norbert Kruse 1, 2, 3
Affiliation  

The interaction of oxygen with a reactive metal is ubiquitous, yet the precise atomic-level mechanisms and pathways leading to the formation of a surface oxide are not well-understood. We report oxygen atom distributions inside Rh single nanoparticles using atom probe microscopy (APM) and demonstrate that mainly facets of the ⟨022̅⟩ crystallographic directions act as oxygen-permeable gateways. The highly anisotropic spatial distribution of incorporated oxygen atoms is in agreement with video-field emission analyses according to which {113} facets of the ⟨022̅⟩ zones act as portals for subsurface diffusion. In addition to providing a more fundamental understanding of the precursor states to metal corrosion, in particular for the case of nanosized metal particles, our studies are also relevant for heterogeneous catalysis where catalytic activity and selectivity conform to reaction-induced structural changes of metal nanoparticles.

中文翻译:

金属氧化的定向途径:3D化学作图揭示了铑纳米颗粒中的氧扩散途径。

氧与反应性金属的相互作用是普遍存在的,但是导致形成表面氧化物的精确的原子级机理和途径尚未得到很好的理解。我们使用原子探针显微镜(APM)报告Rh单个纳米粒子内部的氧原子分布,并证明that022̅⟩晶体学方向的主要刻面起着透氧通道的作用。结合的氧原子的高度各向异性的空间分布与视频场发射分析一致,根据该分析,⟨022̅⟩区的{113}面充当地下扩散的入口。除了提供对金属腐蚀的前体状态(尤其是对于纳米金属颗粒的情况)的更基本的了解之外,
更新日期:2020-04-24
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