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A Structurally Characterized Nonheme Cobalt-Hydroperoxo Complex Derived from Its Superoxo Intermediate via Hydrogen Atom Abstraction
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A Structurally Characterized Nonheme Cobalt-Hydroperoxo Complex Derived from Its Superoxo Intermediate via Hydrogen Atom Abstraction

Chun-Chieh Wang, Hao-Ching Chang, Yei-Chen Lai, Huayi Fang, Chieh-Chin Li, Hung-Kai Hsu, Zong-Yan Li, Tien-Sung Lin, Ting-Shen Kuo, Frank Neese, …
Journal of the American Chemical Society, 卷.138(43), 頁碼.14186-14189
11/2016

摘要

Catalysis Chemistry (all) Biochemistry Colloid and Surface Chemistry
Bubbling O 2 into a THF solution of Co II (BDPP) (1) at -90 °C generates an O 2 adduct, Co(BDPP)(O 2 ) (3). The resonance Raman and EPR investigations reveal that 3 contains a low spin cobalt(III) ion bound to a superoxo ligand. Significantly, at -90 °C, 3 can react with 2,2,6,6-tetramethyl-1-hydroxypiperidine (TEMPOH) to form a structurally characterized cobalt(III)-hydroperoxo complex, Co III (BDPP)(OOH) (4) and TEMPO . Our findings show that cobalt(III)-superoxo species are capable of performing hydrogen atom abstraction processes. Such a stepwise O 2 -activating process helps to rationalize cobalt-catalyzed aerobic oxidations and sheds light on the possible mechanism of action for Co-bleomycin.

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