CAREER: Intelligent Synthesis of Colloidal Nanocrystals Enabled by Microreaction Engineering in Flow

这个CAREER项目的目标是发展基础科学知识，使设计用于合成钙钛矿纳米晶体（量子点）的模块化流动反应器成为可能。目标材料将是卤化铅钙钛矿量子点，它在高效太阳能电池、高清彩色显示器和光催化方面具有潜在的应用前景。该项目将采用模块化流动反应器来研究这些材料的复杂成核和生长机制，并开发必要的工艺-结构-性能关系，以优化合成具有定制性能的钙钛矿量子点。该研究项目将与教育和推广项目相结合，旨在培训研究生和本科生关于流动化学的知识，通过模块化反应器竞赛吸引6-12年级的学生，通过YouTube视频教育公众，并招募代表性不足的群体成员进入STEM职业。该研究将重点研究钙钛矿纳米晶体的成核过程、生长动力学和组成调整，方法是在模块化流动反应器中使用原位监测晶体生长过程来反卷积混合和反应时间。研究了钙钛矿纳米晶成核的基本原理，并在稳定表面配体存在的可控微尺度混合环境下进行了研究。将使用机器学习（ML）增强的工艺优化来研究流动中卤化物交换反应介导的晶体生长和成分调整的反应动力学，以实现窄线宽（90 meV）和高光致发光（PL）量子产率（90%）的发射带隙（1.7至3 eV）的精确调整，从而实现这些材料的商业应用。研究在模块化流动反应器中卤化物交换反应生成的卤化铅钙钛矿纳米晶体的结构（组成）-性能（PL）关系，目的是开发一个按需智能合成具有定制性能的钙钛矿纳米晶体的平台。除了培训一名研究生和两名本科生进行研究外，该项目还将包括研究生和本科生关于流动化学的课程开发，以及针对6-12年级学生、普通公众、与科学与工程女性协会（WISE）和北卡罗莱纳州立大学工程专业即将入学的少数族裔新生暑期过渡项目合作，招募代表性不足的群体成员进入STEM职业。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

The goal of this CAREER project is to develop the fundamental scientific knowledge that will enable the design of modular flow reactors for the synthesis of nanocrystals (quantum dots) of perovskites. The target materials will be lead halide perovskite quantum dots that have potential applications in high-efficiency solar cells, high-definition color displays, and photocatalysis. This project will employ modular flow reactors to study the complex nucleation and growth mechanisms of these materials and develop the necessary process-structure-property relations required for optimal synthesis of perovskite quantum dots with tailored properties. The research program will be integrated with education and outreach programs aimed at training graduate and undergraduate students on flow chemistry, engaging grade 6-12 students through a modular reactor competition, educating the general public through YouTube videos, and recruiting members of underrepresented groups into STEM careers.The proposed research will be focused on studying the nucleation process, growth kinetics and composition tuning of perovskite nanocrystals by deconvoluting the mixing and reaction times in a modular flow reactor using in situ monitoring of the crystal growth process. The fundamentals of perovskite nanocrystal nucleation will be studied under a controlled microscale mixing environment in the presence of stabilizing surface ligands. The reaction kinetics of crystal growth and composition tuning mediated by halide exchange reactions in flow will be studied using machine learning (ML)-enhanced process optimization to achieve precise tuning of emission bandgap (between 1.7 and 3 eV) with narrow linewidth (90 meV and high photoluminescence (PL) quantum yield (90%) to enable commercial applications of these materials. The structure (composition)-property (PL) relationship of lead halide perovskite nanocrystals enabled by halide exchange reactions in the modular flow reactor will be studied with the purpose of developing a platform for on-demand intelligent synthesis of perovskite nanocrystals with tailored properties. In addition to training a graduate student and two undergraduate students in research, the project will involve graduate and undergraduate curriculum development on flow chemistry and outreach activities aimed at grade 6-12 students, the general public, and at recruiting members of underrepresented groups into STEM careers in collaboration with the Women in Science and Engineering (WISE) and the Summer Transition Program for incoming minority freshmen in Engineering at North Carolina State University.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.