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原位液池 STEM 揭示的铂纳米晶成核和生长的多步原子机制。

Multi-step atomic mechanism of platinum nanocrystals nucleation and growth revealed by in-situ liquid cell STEM.

机构信息

Electron Microscopy Center, Empa--Swiss Federal Laboratories for Materials Science and Technology, Überlandstrasse 129, 8600, Dübendorf, Switzerland.

出版信息

Sci Rep. 2021 Dec 14;11(1):23965. doi: 10.1038/s41598-021-03455-w.

Abstract

The understanding of crystal growth mechanisms has broadened substantially. One significant advancement is based in the conception that the interaction between particles plays an important role in the growth of nanomaterials. This is in contrast to the classical model, which neglects this process. Direct imaging of such processes at atomic-level in liquid-phase is essential for establishing new theoretical models that encompass the full complexity of realistic scenarios and eventually allow for tailoring nanoparticle growth. Here, we investigate at atomic-scale the exact growth mechanisms of platinum nanocrystals from single atom to final crystals by in-situ liquid phase scanning transmission electron microscopy. We show that, after nucleation, the nanocrystals grow via two main stages: atomic attachment in the first stage, where the particles initially grow by attachment of the atoms until depletion of the surrounding zone. Thereafter, follows the second stage of growth, which is based on particle attachment by different atomic pathways to finally form mature nanoparticles. The atomic mechanisms underlying these growth pathways are distinctly different and have different driving forces and kinetics as evidenced by our experimental observations.

摘要

晶体生长机制的理解已经大大拓宽。一个重要的进展是基于这样一个概念,即颗粒之间的相互作用在纳米材料的生长中起着重要作用。这与经典模型形成对比,经典模型忽略了这一过程。在液相中进行原子级别的直接成像对于建立新的理论模型至关重要,这些模型涵盖了真实情况下的全部复杂性,并最终允许对纳米颗粒的生长进行定制。在这里,我们通过原位液相扫描透射电子显微镜在原子尺度上研究了从单个原子到最终晶体的铂纳米晶体的确切生长机制。我们表明,在成核之后,纳米晶体通过两个主要阶段生长:在第一阶段通过原子附着,颗粒最初通过原子的附着生长,直到周围区域耗尽。此后,进入第二阶段的生长,其基于通过不同的原子途径进行颗粒附着,最终形成成熟的纳米颗粒。我们的实验观察证明,这些生长途径的原子机制明显不同,具有不同的驱动力和动力学。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d9a9/8671505/abe632c34d9a/41598_2021_3455_Fig1_HTML.jpg

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