CAREER: Rational Design of Dual-Functional Photocatalysts for Synthetic Reactions: Controlling Photosensitization and Reaction with a Single Nanocrystal

在NSF化学部化学催化（CAT）项目的支持下，纽约皇后学院化学与生物化学系的Chen Wang博士正在开发基于钙钛矿纳米晶体的新型催化剂，用于利用光高效合成生物医学和制药应用中必不可少的有机化学品。该项目将采用各种光谱方法来了解纳米晶体中的光生激发态如何转换光能并选择性地促进纳米晶体表面上所需的化学过程。该项目集成了合成化学，物理化学，材料科学和仪器开发，因此将为各级学生提供多学科的学习环境。光化学研究将被引入本科课程，以培养来自不同文化背景的学生。计划开展包括光化学讲习班和暑期研究营在内的外联活动，以接触到K-12学生，并鼓励各种各样的有才华的学生考虑在科学、技术、工程和数学领域进行学习。该项目将探索具有金属卤化物钙钛矿纳米晶体（PNC）的催化平台，目标是实现有效的光敏化和反应控制。该项目将设计PNC表面，以促进重要的合成反应，如环加成和C-C偶联反应，并通过实验和计算研究相结合来了解改性的PNC表面。表面光催化过程将跟踪使用各种超快光谱方法，包括瞬态吸收，时间分辨光致发光，和时间分辨受激共振拉曼光谱。该研究旨在揭示PNC的表面环境与其催化性能之间的关系，以指导基于半导体纳米晶体的新型光催化剂的合理设计。该奖项反映了NSF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。

With support from the Chemical Catalysis (CAT) program of the NSF Division of Chemistry, Dr. Chen Wang of the Department of Chemistry and Biochemistry at Queens College, City University of New York, is developing novel catalysts based on perovskite nanocrystals for utilizing light to efficiently synthesize organic chemicals that are essential in biomedical and pharmaceutical applications. The project will employ various spectroscopic methods to understand how photo-generated excited states in the nanocrystals can convert light energy and selectively promote the desired chemical processes on the nanocrystal surface. The project integrates synthetic chemistry, physical chemistry, materials science, and instrumentation development and hence will provide a multidisciplinary learning environment for students at all levels. Photochemical research will be introduced into the undergraduate curriculum to train students from diverse cultural backgrounds. Outreach activities, including photochemistry workshops and summer research camps, are planned to reach out to K-12 students and encourage a diverse, talented pool of students to consider pursuing studies in science, technology, engineering and mathematics fields.Photocatalytic synthesis has the potential to provide for streamlined, energy-efficient synthetic routes into useful molecules by providing novel bond construction manifolds. The proposed project will explore catalytic platforms with metal halide perovskite nanocrystals (PNCs) with the goals of achieving both efficient photosensitization and reaction control. The project will engineer the PNC surface will the goal of facilitating important synthetic reactions, such as cycloadditions and C-C coupling reactions, and with the goal of understanding the modified PNC surface through a combination of experimental and computational investigation. Surface photocatalytic processes will be tracked using a variety of ultrafast spectroscopic methods, including transient absorption, time-resolved photoluminescence, and time-resolved stimulated resonance Raman spectroscopy. This mechanistic study aims to reveal the relationship between the surface environment of PNCs and their catalytic performance to guide the rational design of novel photocatalysts based on semiconductor nanocrystals.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.