Developing New Molecular Architectures for Devices for Photoinitiated Electron Collection

无机化学、生物无机化学和金属有机化学项目的这一奖项支持弗吉尼亚理工大学化学系的Karen J.Breyer博士对超分子无机络合物开发的研究。将合成包含扩展光吸收有机部分的过渡金属系统，并测试它们促进光引发的多电子转移的能力。基本的分子设计将包括将两个光吸收体耦合到一个中心的、催化活性的金属中心，该中心将作为电子的收集位置。光吸收系统将是多金属的，并被设计为具有基于金属的最高占据分子轨道，这些分子轨道定位在分子的外围，与最低未占据分子轨道定位的中心位置很好地分开。然后，遥远的金属中心将作为中央电子收集核心的电子供体。这些系统的光谱和电化学性质的细节将被确定并用于优化设计。将光能转化为化学能的材料是开发太阳能设备所必需的。在理想的条件下储存和传输许多电子是一个重要的目标。许多自然过程，如二氧化碳的减少和固氮，都需要许多电子。在这个基础研究项目中，将合成一些新的多金属化合物，并测试它们吸收光能和释放大量电子用于化学反应的效率。

This award in the Inorganic, Bioinorganic, and Organometallic Chemistry Program supports research on development of supramolecular inorganic complexes by Dr. Karen J. Brewer of the Chemistry Department, Virginia Polytechnic University. Transition metal systems containing extended light-absorbing organic moieties will be synthesized and tested for their ability to facilitate photoinitiated multielectron transfer. The basic molecular design will involve the coupling of two light absorbers to a central, catalytically active metal center that will serve as the site of collection of the electrons. The light absorber systems will be multimetallic and designed to have metal-based highest occupied molecular orbitals that are localized on the periphery of the molecules, well separated from the central site of localization of the lowest unoccupied molecular orbital. The remote metal centers will then function as electron donors for the central electron collecting core. Details of the spectroscopic and electrochemical properties of these systems will be determined and used to optimize the design. Materials that convert light energy to chemical energy are necessary for development of solar energy devices. Storage and delivery of many electrons under desired conditions is an important goal. Many natural processes such as the reduction of carbon dioxide and nitrogen fixation require many electrons. In this fundamental research project, some new multi-metal compounds will be synthesized and tested for their efficiency in absorbing light energy and in releasing many electrons for use in chemical reactions.