CAREER: Tetrapyrrole Architectures Displaying a Multielectron Redox Chemistry for CO2 Activation and Energy Catalysis

在这个由化学系化学催化计划资助的项目中，特拉华大学的乔尔·罗森塔尔教授将为小分子物种的活化和相互转化开发新的催化剂平台。具有能源后果的过程将成为目标。这项研究将集中在合成和研究具有特殊光物理和多电子氧化还原性质的新的四吡咯配合物。这些系统将通过X射线结晶学、伏安法和几种类型的电子光谱的组合进行彻底检查。将使用电化学和化学还原方法来探索四吡咯配合物催化氧还原反应和二氧化碳转化为化学燃料的能力。该职业奖还支持通过在特拉华大学的暑期研究实习来提高高中生接触无机化学和能源科学的机会。这项工作的更广泛影响包括开发能够促进可再生能源转换和从二氧化碳生产燃料的廉价催化剂的潜在社会效益。此外，该项目将为新一代个人提供指导、教育和培训，使他们为迎接21世纪的科学和社会挑战做好准备。该项目的重点是开发新的无机平台，这些平台可以驱动对能量储存和转换至关重要的化学转化。为了迎接这一挑战，人们将制备、表征和研究比传统金属络合物更便宜、更容易获得的新的金属络合物。这项研究还将展示这些廉价的分子平台促进涉及小分子的化学转化中所需的具有挑战性的成键和断裂过程的能力。一些具体目标包括开发将二氧化碳转化为燃料的催化剂。

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Joel Rosenthal of the University of Delaware will develop new catalyst platforms for the activation and interconversion of small molecule species. Processes that have energy consequences will be targeted. This research will focus on the synthesis and study of new tetrapyrrole complexes with unusual photophysical and multielectron redox properties. These systems will be thoroughly examined by a combination of X-ray crystallography, voltammetry and several types of electronic spectroscopy. Electrochemical and chemical reduction methods will be used to probe the ability of the tetrapyrrole complexes to catalyze the oxygen reduction reaction and the conversion of carbon dioxide to chemical fuels. This CAREER award also supports outreach to improve the accessibility of inorganic chemistry and energy science to high school students via summer research internships at the University of Delaware. The broader impacts of this work include potential societal benefits from the development of inexpensive catalysts that can promote renewable energy conversion and production of fuels from carbon dioxide. Additionally, the project will provide mentorship, education and training of a new generation of individuals in order to prepare them for the scientific and societal challenges of the 21st century. This project focuses on the development of new inorganic platforms that can drive chemical transformations that are important for energy storage and conversion. To meet this challenge, new metal complexes that are less expensive and easier to obtain than conventional ones will be prepared, characterized and studied. This research will also demonstrate the ability of these inexpensive molecular platforms to promote the challenging bond making and breaking processes that are required in chemical conversions involving small molecules. Some specific goals include developing catalysts for the conversion of carbon dioxide into fuels.