SusChEM: Hydrogen Chemistry of Earth Abundant Metals

化学系化学合成（SYN）项目的这个奖项支持华盛顿大学化学系Michael Heinekey教授的一个项目。该项目将探索氢的化学性质。氢有潜力成为一种重要的运输燃料和我们能源基础设施的重要组成部分。铂和相关金属的成本和供应有限阻碍了这一领域的进展，而铂和相关金属是目前催化氢生产和利用的首选材料。该项目将探索使用更便宜和更丰富的金属，如铁、镍和钴。该项目还将为本科生和研究生提供优秀的跨学科培训，包括那些来自历史上在科学领域代表性不足的群体的学生。它将允许Heinekey教授和学生继续参与针对公众的外展活动。将探索氢活化的仿生方法，最近发现的氢化酶活性位点结构提供了灵感。模型配合物将由一个铁中心，两个铁中心和铁/镍对，以及适当的共配体，包括一氧化碳和异腈配体制备。氢与这些配合物的结合将作为酶的氧化形式的模型来研究。氢与铁和镍配合物结合的进一步研究将进行，以阐明质子从结合氢转移到各种碱的机制。二氢，末端氢化物和桥接氢化物配体的相互转化也将作为氢被氢化酶激活的模型进行研究。氢配合物还将作为氟利昂中碳氯键氢解的催化剂进行研究，这可能会导致回收这些消耗臭氧的分子的实际过程。

This award in the Chemical Synthesis (SYN) program in the Division of Chemistry supports a project by Professor Michael Heinekey in the Department of Chemistry at the University of Washington. The project will explore the chemistry of hydrogen. Hydrogen has the potential to become a significant transportation fuel and an important part of our energy infrastructure. Progress in this area has been hindered by the cost and limited supply of platinum and related metals, which are the current materials of choice for catalysis of hydrogen production and utilization. This project will explore the use of less expensive and more abundant metals such as iron, nickel and cobalt. This project will also provide excellent interdisciplinary training of undergraduate and graduate students, including those from groups historically underrepresented in the sciences. It will allow both Professor Heinekey and students to continue to participate in outreach activities directed to the general public.Biomimetic approaches to hydrogen activation will be explored, with inspiration provided by the recently discovered active site structures of hydrogenase enzymes. Model complexes will be prepared with one iron center, two iron centers and iron/nickel pairs, along with appropriate co-ligands, including carbon monoxide and isonitrile ligands. The binding of hydrogen to these complexes will be studied as a model for the oxidized form of the enzyme.Additional studies of hydrogen binding to iron and nickel complexes will be undertaken to elucidate the mechanism of proton transfer from bound hydrogen to various bases. Interconversion of dihydrogen, terminal hydride and bridging hydride ligands will also be investigated as a model for the activation of hydrogen by the hydrogenase enzymes. Hydrogen complexes will also be studied as catalysts for the hydrogenolysis of carbon chlorine bonds in Freons, which may lead to practical processes for recycling of these ozone depleting molecules.