Coordination Complexes with Multiple Inorganic Functional Groups

该奖项由美国国家科学基金会化学合成项目资助，支持威斯康星大学麦迪逊分校John F. Berry研究小组的工作，该小组旨在利用多个无机官能团促进多电子过程。这里，“无机官能团”被定义为能够进行至少一种氧化还原反应的单位。因此，结合多个官能团应该导致观察到多个氧化还原反应可用于同一分子。例如，具有Mo(II)-Mo（II）四键官能团的化合物可以经过双电子氧化生成三键Mo(III)-Mo(III)，金属-氧官能团可以经过双电子氧原子转移过程。这两个官能团可以这样一种方式结合，允许可逆的四电子氧化还原和o原子转移反应发生。在这项工作中，结合无机官能团的化合物的探索将为发现新的多电子反应提供一条途径。要研究的无机官能团的范围从金属-金属多键，包括金属氧、碳和氮化合物，到每一种金属作为一个单独的官能团的杂金属物种。多电子反应在化学和生物过程中都是非常重要的。例如，分子（如分子氧）的多电子还原不仅在生物学上具有重要意义，发生在有氧呼吸中，而且在重要的能源相关技术中起着关键作用，如燃料电池和水分解。提高这种多电子反应的效率是化学领域面临的一个基本挑战。促进多电子化学的新方法具有重要意义，该奖项支持旨在发现新的多电子反应的概念进步。这一进展包括将不同的过渡金属化合物的特性结合起来，每个化合物都能进行电子转移，形成能够进行多电子转移的新化合物。

This award funded through the NSF Chemical Synthesis program supports work in the research group of John F. Berry at the University of Wisconsin--Madison aimed at using multiple inorganic functional groups to promote multi-electron processes. Here an "inorganic functional group" is defined as a unit capable of at least one redox reaction. Thus, combining multiple functional groups should lead to the observation of multiple redox reactions available to the same molecule. For example, a compound having a Mo(II)-Mo(II) quadruple bond 'functional group' can undergo two-electron oxidation to yield a triply-bonded Mo(III)-Mo(III) species, and a metal-oxo 'functional group' can undergo two-electron oxygen atom transfer processes. These two functional groups can be combined in such a way as to permit reversible four-electron redox and O-atom transfer reactions to take place. In this work, the exploration of compounds that combine inorganic functional groups will provide a pathway towards the discovery of new multi-electron reactions. The inorganic functional groups to be studied range from metal-metal multiple bonds, including metal oxo, carbene, and nitrido compounds, to heterometallic species in which each metal serves as a separate functional group.Multi-electron reactions are very important in chemistry as well as in biological processes. For example, multi-electron reductions of molecules such as molecular oxygen are not only biologically important, occurring in aerobic respiration, but also play key roles in important energy-related technologies, such as fuel cells and water splitting. A fundamental challenge in the chemical community is to improve the efficiency of such multi-electron reactions. New ways to facilitate multielectron chemistry are of great significance, and this award supports a conceptual advance aimed toward the discovery of new multi-electron reactions. This advance involves combining traits of different transition metal compounds, each individually capable of electron transfer, into new compounds able to perform multi-electron transfer.