RUI: Dialing in on the proton: Understanding the role of the proton in photo-induced, proton-coupled electron transfer using tunable model systems

在本研究在本科院校（RUI）项目资助的化学结构，动力学机制B计划的化学部，教授伊丽莎白R。阿默斯特学院化学系的杨教授正在研究模型分子系统中的电子转移。这些模型受到生物系统的启发，特别是蛋白质，它们非常有效地进行生命所必需的反应。这项研究的结果可能会导致更节能的反应的发展，包括将水分解为氢和氧用于能量储存，农业固氮和减少二氧化碳以减少大气中的温室气体。 本科生进行研究，直接参与研究项目的每个阶段：实验设计，物理评估，表征，数据分析和科学写作。学生接受广泛的科学技术培训，并学习尖端研究。此外，该项目还加强了马萨诸塞州先锋谷的研究基础设施。质子耦合电子转移（PCET）驱动了自然系统中的许多关键反应，包括光合作用的捕光反应。本计画将探讨PCET机制研究中的几个特徴。电子转移驱动力和质子转移能力的酸基团在一系列的供体和受体系统之间的相互作用进行了研究，以提供直接洞察氢键界面如何调节电子转移。需要回答的具体问题包括：在哪些电子转移驱动力范围内，质子转移能力会对观察到的速率产生实质性差异？质子在界面内的能力是否导致相同供体和受体部分之间的电子转移速率的显著调制？超分子给体-受体组装方式对偶联和电子转移速率有显著影响吗？这些对PCET的机理研究提供了重要的见解，即光如何被用来引发质子和电子协同运动所促进的化学反应。

In this Research at Undergraduate Institutions (RUI) project funded by the Chemical Structure, Dynamic & Mechanism B Program of the Chemistry Division, Professor Elizabeth R. Young of the Department of Chemistry at Amherst College is studying electron transfer in model molecular systems. These models are inspired by biological systems, specifically proteins, which carry out reactions necessary for life very efficiently. Results of this research could lead to the development of more energy efficient reactions, including splitting water into hydrogen and oxygen for energy storage, nitrogen fixation for agriculture and carbon dioxide reduction to decrease greenhouse gases in the atmosphere. Undergraduate students carry out the research, directly participating in each phase of the research projects: experimental design, physical evaluation, characterization, data analysis and scientific writing. Students are trained in a broad range of scientific techniques and learn cutting-edge research. Additionally, this project enhances the research infrastructure in the Pioneer Valley of Massachusetts. Proton-coupled electron transfer (PCET) drives numerous critical reactions in natural systems, including the light-harvesting reactions of photosynthesis. This project explores several features in the mechanistic study of PCET. The interplay between electron transfer driving force and the proton transfer ability of acid groups in a series of donor and acceptor systems is studied, in order to provide direct insight into how hydrogen-bonded interfaces modulate electron transfer. Specific questions to be answered include: For which electron transfer driving force ranges does the proton transfer ability make a substantial difference in the observed rates? Does the ability of a proton within the interface result in significant modulation in the electron transfer rate between the same donor and acceptor moieties? Does the mode of supramolecular donor-acceptor assembly have a significant impact on coupling and electron transfer rates? These mechanistic studies of PCET provide important insights into how light could be used to initiate chemical reactions that are facilitated by the concerted movement of protons and electrons.