Metal Nanocrystal Formation during Liquid Phase Transmission Electron Microscopy: Thermodynamics and Kinetics of Precursor Conversion, Nucleation, and Growth†,Chemistry of Materials

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Metal Nanocrystal Formation during Liquid Phase Transmission Electron Microscopy: Thermodynamics and Kinetics of Precursor Conversion, Nucleation, and Growth†
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-07-24 , DOI: 10.1021/acs.chemmater.0c01360
Taylor J. Woehl ₁

Affiliation

Colloidal nanoparticle synthesis involves a complex combination of physical and chemical processes that transform a liquid phase metal precursor into nanoparticles, each containing thousands to millions of atoms. Liquid phase transmission electron microscopy (LP-TEM) has enabled unprecedented atomic and nanoscale insights into mechanisms for colloidal nanoparticle formation and promises to unravel many of these complex processes. Despite intense sustained interest in this area, practical translation of LP-TEM mechanistic insights to improve upon and discover new nanomaterial synthesis approaches remains a major unmet challenge. One underlying reason for this is a poor fundamental understanding of how nanocrystal formation during LP-TEM compares to conventional flask-based synthesis. In this perspective, we discuss the fundamental thermodynamic and kinetic driving forces for metal nanocrystal formation during LP-TEM and compare them with established mechanisms for flask-based synthesis. The roles of electron beam induced solution chemistry and nanoscale solute transport phenomena in mediating precursor reduction, nanocrystal nucleation, and growth will be discussed. The recent discovery that the liquid cell enclosure membrane surface chemistry has a significant impact on nanocrystal nucleation mechanisms during LP-TEM will be highlighted. Increasingly quantitative, statistically relevant, and reproducible LP-TEM experiments together with rigorous comparisons to flask-based chemistry are expected to provide new insights into nanocrystal formation mechanisms that are directly relevant to flask-based synthesis.

中文翻译：

液相透射电子显微镜下金属纳米晶体的形成：前体转化，成核和生长的热力学和动力学†

胶体纳米颗粒的合成涉及物理和化学过程的复杂结合，这些过程将液相金属前体转变成纳米颗粒，每个纳米颗粒包含数千至数百万个原子。液相透射电子显微镜（LP-TEM）已使胶体纳米颗粒形成机理获得了前所未有的原子和纳米级见解，并有望解开许多这些复杂的过程。尽管对该领域持续存在着浓厚的兴趣，但为进一步改进和发现新的纳米材料合成方法而进行的LP-TEM机理见解的实用翻译仍然是主要的挑战。造成这种情况的一个潜在原因是，与传统的烧瓶合成方法相比，对LP-TEM过程中纳米晶体形成的基本了解不足。从这个角度来看，我们讨论了在LP-TEM过程中形成金属纳米晶体的基本热力学和动力学驱动力，并将它们与基于烧瓶的合成方法建立的机理进行了比较。将讨论电子束诱导溶液化学和纳米级溶质传输现象在介导前驱体还原，纳米晶体成核和生长中的作用。液体细胞包裹膜表面化学对LP-TEM过程中对纳米晶体成核机制有重大影响的最新发现将被重点介绍。越来越多的定量，统计相关和可重现的LP-TEM实验，以及与瓶型化学的严格比较，有望为与瓶型合成直接相关的纳米晶体形成机理提供新的见解。

更新日期：2020-09-22

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