Organometallic Functionalization of Colloidal Nanocrystal Surfaces for Catalysis

在化学系化学催化项目的支持下，圣母大学的艾米丽崔将研究利用光加速重要化学转化的新方法。具有半导体性质的纳米材料长期以来一直被研究用于光诱导化学转变。然而，精确测量和控制这些材料的表面性质的化学反应性是很难实现的实验。该项目将专注于使用附着在吸光纳米颗粒上的金属中心来提供有关纳米颗粒性质的信息，并作为重要催化转化的反应中心，如碳-碳键形成反应。从这些研究中获得的结果将指导新的光促进反应的发展。这笔赠款还将支持研究生和本科生在这一跨学科领域的研究培训。徐教授的研究团队将积极参与有本地小学生参与的外展活动，重点发展以纳米材料为基础的化学教育单元。研究生和徐博士还将制作有关电化学和催化的实用主题的教育视频，并将在网上免费提供给公众。在这些研究中，艾米丽徐和她在圣母大学的团队将研究使用有机金属羰基碎片配位到半导体量子点的表面进行光催化反应。量子点由于其可调的光吸收特性而被作为许多反应的光敏剂和光催化剂，但是关于表面化学对这些转化的影响仍然存在许多问题。Tsui小组将探索使用表面结合的金属羰基片段作为量子点表面效应的光谱报告者，包括表面偶极矩，这可以与光催化相关的性质，如带边电位。这些光谱特征的定量模型的发展，预计将导致更详细的了解如何表面效应有助于量子点的反应性在光氧化还原转换。此外，徐博士将研究使用表面结合的有机金属碎片作为光催化转化过程中的催化中心。研究生将接受有机金属化学和材料表征方法的培训，为他们提供具有专业价值的跨学科经验。这些学生还将通过参与外展活动和准备一系列电化学视频来进行科学交流方面的培训，这些视频将在网上传播。该奖项反映了NSF的法定使命，并被认为值得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来支持。

With the support of the Chemical Catalysis program in the Division of Chemistry, Emily Tsui of the University of Notre Dame will study new ways of using light to accelerate important chemical transformations. Nanomaterials with semiconductor properties have long been studied for light-induced chemical transformations. However, the precise measurement and control of the surface properties of these materials for chemical reactivity are difficult to achieve experimentally. The project will focus on using metal centers attached to light-absorbing nanoparticles to provide information about the properties of the nanoparticles, and to act as reaction centers for important catalytic transformations such as carbon-carbon bond formation reactions. The results obtained from these studies will guide the development of new light-promoted reactions. This grant will also support the research training of graduate and undergraduate students in this interdisciplinary field. Professor Tsui’s research team will actively participate in outreach activities involving local elementary school students, with a focus on developing educational modules on nanomaterials-based chemistry. Educational videos on practical topics in electrochemistry and catalysis will also be produced by the graduate students and Dr. Tsui, and will made freely available online to the general public.In these studies Emily Tsui and her team at the University of Notre Dame will study the use of organometallic metal carbonyl fragments coordinated to the surfaces of semiconductor nanocrystal quantum dots for photocatalytic reactions. Quantum dots have been targeted as photosensitizers and photocatalysts for many reactions due to their tunable light-absorbing properties, but many questions remain regarding the effects of surface chemistry upon these transformations. The Tsui group will explore the use of surface-bound metal carbonyl fragments to act as spectroscopic reporters of quantum dot surface effects including the surface dipole moment, which can correlate to photocatalytically-relevant properties such as band edge potentials. The development of a quantitative model of these spectroscopic features is expected to lead to a more detailed understanding of how surface effects contribute to quantum dot reactivity during photoredox transformations. Additionally, Dr. Tsui will study the use of the surface-bound organometallic fragments to act as catalytic centers during photocatalytic transformations. Graduate students will be trained in both organometallic chemistry and materials characterization methods, providing them interdisciplinary experience that will be professionally valuable. These students will also be trained in scientific communication through participation in outreach activities and in the preparation of a series of electrochemistry videos that will be disseminated online.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.