高价态锰(IV)-氧-铈(IV)配合物及其增强的氧化反应活性。
A High-Valent Manganese(IV)-Oxo-Cerium(IV) Complex and Its Enhanced Oxidizing Reactivity.
机构信息
Department of Chemistry and Nano Science, Ewha Womans University, Seoul, 03760, Korea.
Department of Physics and Astronomy, Purdue University, 525 Northwestern Ave., West Lafayette, IN, 47907, USA.
出版信息
Angew Chem Int Ed Engl. 2019 Nov 4;58(45):16124-16129. doi: 10.1002/anie.201910032. Epub 2019 Sep 24.
A mononuclear nonheme manganese(IV)-oxo complex binding the Ce ion, [(dpaq)Mn (O)] -Ce (1-Ce ), was synthesized by reacting [(dpaq)Mn (OH)] (2) with cerium ammonium nitrate (CAN). 1-Ce was characterized using various spectroscopic techniques, such as UV/Vis, EPR, CSI-MS, resonance Raman, XANES, and EXAFS, showing an Mn-O bond distance of 1.69 Å with a resonance Raman band at 675 cm . Electron-transfer and oxygen atom transfer reactivities of 1-Ce were found to be greater than those of Mn (O) intermediates binding redox-inactive metal ions (1-M ). This study reports the first example of a redox-active Ce ion-bound Mn -oxo complex and its spectroscopic characterization and chemical properties.
单核非血红素锰(IV)-氧配合物[(dpaq)Mn (O)] -Ce （1-Ce ）与硝酸铈铵（CAN）反应合成，其中 Ce 离子与单核非血红素锰(IV)-氧配合物结合。使用各种光谱技术，如 UV/Vis、EPR、CSI-MS、共振拉曼、XANES 和 EXAFS，对 1-Ce 进行了表征，结果表明 Mn-O 键距离为 1.69 Å，共振拉曼带位于 675 cm 处。发现 1-Ce 的电子转移和氧原子转移反应活性大于结合氧化还原惰性金属离子（1-M ）的 Mn (O) 中间体。本研究报道了首例氧化还原活性 Ce 离子结合的 Mn -氧配合物及其光谱表征和化学性质。
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