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

在这个由化学部化学催化项目资助的项目中，特拉华大学的Joel Rosenthal教授将开发新的催化剂平台，用于小分子物种的活化和相互转化。具有能量后果的过程将成为目标。本课题将重点研究具有特殊光物理性质和多电子氧化还原性质的新型四吡咯配合物的合成和研究。这些系统将通过x射线晶体学、伏安法和几种电子光谱学的结合进行彻底的检查。电化学和化学还原方法将用于探测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，提高高中学生对无机化学和能源科学的可及性。这项工作的更广泛影响包括开发廉价催化剂的潜在社会效益，这些催化剂可以促进可再生能源的转化和从二氧化碳中生产燃料。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21世纪的科学和社会挑战做好准备。该项目侧重于开发新的无机平台，这些平台可以驱动对能量存储和转换很重要的化学转化。为了应对这一挑战，人们将制备、表征和研究比传统金属更便宜、更容易获得的新型金属配合物。这项研究还将证明这些廉价的分子平台在促进涉及小分子的化学转化所需的具有挑战性的键形成和断裂过程中的能力。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.