Elucidating the weakly reversible Cs-Pb-Br perovskite nanocrystal reaction network with high-throughput maps and transformations,Journal of the American Chemical Society

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Elucidating the weakly reversible Cs-Pb-Br perovskite nanocrystal reaction network with high-throughput maps and transformations
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-06-12 , DOI: 10.1021/jacs.0c04997
Jakob C Dahl , Xingzhi Wang , Xiao Huang , Emory M Chan , A Paul Alivisatos ₁

Affiliation

Advances in automation and data analytics can aid exploration of the complex chemistry of nanoparticles. Lead halide perovskite colloidal nanocrystals provide an interesting proving ground: there are reports of many different phases and transformations, which has made it hard to form a coherent conceptual framework for their controlled formation through traditional methods. In this work, we systematically explore the portion of Cs-Pb-Br synthesis space in which many optically distinguishable species are formed using high-throughput robotic synthesis to understand their formation reactions. We deploy an automated method that allows us to determine the relative amount of absorbance that can be attributed to each species in order to create maps of the synthetic space. These in turn facilitate improved understanding of the interplay between kinetic and thermodynamic factors that underlie which combination of species are likely to be prevalent under a given set of conditions. Based on these maps, we test potential transformation routes between perovskite nanocrystals of different shapes and phases. We find that shape is determined kinetically, but many reactions between different phases show equilibrium behavior. We demonstrate a dynamic equilibrium between complexes, monolayers and nanocrystals of lead bromide, with substantial impact on the reaction outcomes. This allows us to construct a chemical reaction network that qualitatively explains our results as well as previous reports and can serve as a guide for those seeking to prepare a particular composition and shape.

中文翻译：

用高通量图谱和转换阐明弱可逆的 Cs-Pb-Br 钙钛矿纳米晶反应网络

自动化和数据分析的进步可以帮助探索纳米粒子的复杂化学。卤化铅钙钛矿胶体纳米晶体提供了一个有趣的试验场：有许多不同的相和转变的报道，这使得很难通过传统方法为其受控形成形成一个连贯的概念框架。在这项工作中，我们系统地探索了 Cs-Pb-Br 合成空间的一部分，其中使用高通量机器人合成形成了许多光学可区分的物种，以了解它们的形成反应。我们部署了一种自动化方法，使我们能够确定可归因于每个物种的吸光度的相对量，以创建合成空间的地图。这些反过来又促进了对动力学和热力学因素之间相互作用的更好理解，这些因素是在给定条件下可能普遍存在的物种组合的基础。基于这些图，我们测试了不同形状和相的钙钛矿纳米晶体之间的潜在转化路线。我们发现形状是由动力学决定的，但不同相之间的许多反应显示出平衡行为。我们证明了溴化铅的复合物、单层和纳米晶体之间的动态平衡，对反应结果有重大影响。这使我们能够构建一个化学反应网络，定性地解释我们的结果以及以前的报告，并可以作为那些寻求准备特定成分和形状的人的指南。

更新日期：2020-06-12

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