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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(42):13078-13082
The robust, high‐valent NiIV complex [(Py)2NiIVF2(CF3)2] (Py=pyridine) was synthesized and fully characterized by NMR spectroscopy, X‐ray diffraction, and elemental analysis. It reacts with aromatic compounds at 25 °C to form the corresponding benzotrifluorides in nearly quantitative yield. The monomeric and dimeric NiIIICF3 complexes 2 ⋅Py and 2 were identified as key intermediates, and their structures were unambiguously determined by EPR spectroscopy and X‐ray diffraction. Preliminary kinetic studies in combination with the isolation of reaction intermediates confirmed that the C−H bond‐breaking/C−CF3 bond‐forming sequence can occur both at NiIVCF3 and NiIIICF3 centers. 相似文献
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Deepika G. Karmalkar Muniyandi Sankaralingam Mi Sook Seo Roman Ezhov Yong‐Min Lee Yulia N. Pushkar Won‐Suk Kim Shunichi Fukuzumi Wonwoo Nam 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(45):16270-16275
A mononuclear nonheme manganese(IV)–oxo complex binding the Ce4+ ion, [(dpaq)MnIV(O)]+–Ce4+ ( 1 ‐Ce4+), was synthesized by reacting [(dpaq)MnIII(OH)]+ ( 2 ) with cerium ammonium nitrate (CAN). 1 ‐Ce4+ 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?1. Electron‐transfer and oxygen atom transfer reactivities of 1 ‐Ce4+ were found to be greater than those of MnIV(O) intermediates binding redox‐inactive metal ions ( 1 ‐Mn+). This study reports the first example of a redox‐active Ce4+ ion‐bound MnIV‐oxo complex and its spectroscopic characterization and chemical properties. 相似文献
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