Devi Tarali, Lee Yong-Min, Nam Wonwoo, Fukuzumi Shunichi
Department of Chemistry and Nano Science, Ewha Womans University, Seoul 03760, Korea.
Chem Commun (Camb). 2019 Jul 11;55(57):8286-8289. doi: 10.1039/c9cc03245b.
The chemistry of metal-superoxo intermediates started being unveiled in oxidation reactions by enzymes and their synthetic model compounds. However, aromatic hydroxylation reactions by the metal-superoxo species are yet to be demonstrated. In this study, we report for the first time that the hydroxylation of aromatic compounds such as anthracene and its derivatives by a mononuclear nonheme Cr(iii)-superoxo complex, [(Cl)(TMC)CrIII(O2)]+ (1), occurs in the presence of triflic acid (HOTf) via the rate-determining proton-coupled electron transfer (PCET) from anthracene to 1, followed by a fast further oxidation to give anthraquinone. The rate constants of electron transfer from anthracene derivatives to 1 in the presence of HOTf are well analyzed in light of the Marcus theory of electron transfer.
金属超氧中间体的化学性质开始在酶及其合成模型化合物的氧化反应中得以揭示。然而,金属超氧物种引发的芳香族羟基化反应尚未得到证实。在本研究中,我们首次报道,在三氟甲磺酸(HOTf)存在下,单核非血红素Cr(III)-超氧配合物[(Cl)(TMC)CrIII(O2)]+(1)会使蒽及其衍生物等芳香族化合物发生羟基化反应,该反应通过从蒽到1的速率决定步骤——质子耦合电子转移(PCET)进行,随后快速进一步氧化生成蒽醌。根据马库斯电子转移理论,对在HOTf存在下蒽衍生物向1的电子转移速率常数进行了很好的分析。