Robot-Accelerated Perovskite Investigation and Discovery
Robot-Accelerated Perovskite Investigation and Discovery
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DOI：
10.1021/acs.chemmater.0c01153
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发表时间：
2020-07-14
影响因子：
8.6
通讯作者：
Chan, Emory M.
中科院分区：
文献类型：
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作者：
Li, Zhi;Najeeb, Mansoor Ani;Chan, Emory M.
金属卤化物钙钛矿材料是一类很有前途的新一代光伏和光电子器件材料。新的钙钛矿衍生材料的发现和全面表征受到单晶X射线衍射研究所需的高质量晶体生长困难的限制。我们提出了一种基于逆温结晶(ITC)的自动化、高通量的金属卤化物钙钛矿单晶发现方法，作为一种快速识别和优化合成条件以形成高质量单晶的手段。使用这种自动化方法，总共进行了8172个金属卤化物钙钛矿合成反应，反应使用了45个有机铵离子。这种机器人筛选将ITC合成路线可获得的金属卤化物钙钛矿材料的数量增加了5倍以上，并导致了两个新相的形成，[C2H7N2][PbI3]和[C7H16N](2)[PbI4]。这一综合数据集允许对整个实验空间和形成大单晶的可能性进行统计量化。此外，该数据集使构建和评估用于预测晶体形成条件的机器学习模型成为可能。这项工作是一项概念验证，将高通量实验和机器学习相结合，加速和加强了金属卤化物钙钛矿结晶的研究。这种方法被设计成可推广到不同的合成路线，以加速材料的发现。
Metal halide perovskites are a promising class of materials for next-generation photovoltaic and optoelectronic devices. The discovery and full characterization of new perovskite-derived materials are limited by the difficulty of growing high quality crystals needed for single-crystal Xray diffraction studies. We present an automated, high-throughput approach for metal halide perovskite single crystal discovery based on inverse temperature crystallization (ITC) as a means to rapidly identify and optimize synthesis conditions for the formation of high quality single crystals. Using this automated approach, a total of 8172 metal halide perovskite synthesis reactions were conducted using 45 organic ammonium cations. This robotic screening increased the number of metal halide perovskite materials accessible by an ITC synthesis route by more than 5-fold and resulted in the formation of two new phases, [C2H7N2][PbI3] and [C7H16N](2)[PbI4]. This comprehensive data set allows for a statistical quantification of the total experimental space and of the likelihood of large single crystal formation. Moreover, this data set enables the construction and evaluation of machine learning models for predicting crystal formation conditions. This work is a proof-of-concept that combining high throughput experimentation and machine learning accelerates and enhances the study of metal halide perovskite crystallization. This approach is designed to be generalizable to different synthetic routes for the acceleration of materials discovery.