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제125회 대한화학회 학술발표회 및 총회 Synthesis and Characterization of Triiron-phosphide complexes

2020년 2월 6일 13시 45분 23초
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화 11시 : 20분
Inorganic Chemistry - Emerging Researchers in Inorganic Chemistry
저자 및
Jaesung Kwak
Green Carbon Catalysis Research Center, Korea Research Institute of Chemical Technology, Korea
The synthesis of polynuclear metal complexes has drawn significant interest recently. These expanded redox reservoirs in the polynuclear core of these clusters have the capability to cooperatively activate small molecules. Many of these systems are inspired by metalloenzyme cofactors or heterogeneous surfaces. One of the structural features of these clusters is utilizing a single atom adduct as a bridging component between transition metal centers (such as C- or S- atoms in FeMo-cofactor in nitrogenase). It has been hypothesized that the single atom ligands play a larger role than just structural features, and may also be involved in the redox properties of the clusters. We have developed a family of hexaamide based ligand scaffold comprised of o-phenylenedianalide moieties to proximally coordinate three divalent metal ions, resulting in a trinuclear core with a variety of metal centers (Fe, Co, Mn, Ni, etc). We have synthesized a sterically encumbered variant utilizing t-butyldimethylsilyl groups, 1,3,5-C6H9(NHC6H4-o-NHSiMe2tBu)3 (tbsLH6) and can generate the triiron cluster (tbsL)Fe3(thf) in a maximally high-spin ground state (S=6). The rich redox chemistry of these clusters has been investigated, and they have been shown to promote multi-electron transfer reactions. This work will describe our efforts to introduce a heavier pnictogen (P) atom and the stability it provides to the cluster across a range of oxidation states. In addition, interesting reactivity on single phosphorus atom will be included.