Synthesis and Stabilization of High-Oxidation State Metal Complexes: Opportunities for Novel Structure and Reactivity

化学合成(SYN)项目的这一奖项支持加州大学圣巴巴拉分校的Trevor W.Hayton教授开展关于金属离子在其最高氧化态的合成和反应性的基础研究。通常，高氧化态的络合物活性太高，难以分离，这使得它们的表征和研究成为一个重大挑战。因此，我们正在尝试新的方法，无论是在配体设计方面，还是在合成方法方面，以促进高价金属离子的化学。具体地说，我们正在开发能够稳定这些氧化态的强电子供体配体，如ketimide配体。同样，我们正在开发新的、广泛适用的合成路线，以产生金属-配体多键。为了实现后一个目标，我们正在利用保护/去保护方法来获得这些新的官能团。该奖项资助的基础研究将推进高氧化态材料的合成操作，并提供对离子反应性的更多了解。其中许多离子，特别是锰和铁，在催化和人工光合作用方面有潜在的应用，我们获得的信息将用于缓解我们日益严重的能源短缺。

This award in the Chemical Synthesis (SYN) program supports work by Professor Trevor W. Hayton at the University of California Santa Barbara to carry out fundamental studies on the synthesis and reactivity of metal ions in their highest oxidation states. Often complexes in high oxidation states are too reactive to isolate, making their characterization and study a significant challenge. Thus we are trying new approaches, both in terms of ligand design and synthetic methodologies, to advance the chemistry of high valent metal ions. Specifically, we are developing strongly electron donating ligands, such as the ketimide ligand, which are capable of stabilizing these oxidation states. In a similar vein, we are developing new, broadly applicable synthetic routes for generating metal-ligand multiple bonds. To realize this latter goal we are utilizing the protection/deprotection methodology to access these novel functional groups. The basic research funded by this award will advance the synthetic manipulation of high oxidation state materials and provide a greater understanding of the reactivity of ions. Many of these ions, in particular, manganese and iron, have potential applications in catalysis and artificial photosynthesis, and the information we acquire will be used in efforts to alleviate our growing energy shortage.