Involvement of a Formally Copper(III) Nitrite Complex in Proton-Coupled Electron Transfer and Nitration of Phenols

铜(III)亚硝酸盐络合物参与质子耦合电子转移和酚的硝化反应

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Abstract

A unique high-valent copper nitrite species, LCuNO(2), was accessed via the reversible one-electron oxidation of [M][LCuNO(2)] (M = NBu(4)(+) or PPN(+)). The complex LCuNO(2) reacts with 2,4,6-tri-tert-butylphenol via a typical proton-coupled electron transfer (PCET) to yield LCuTHF and the 2,4,6-tri-tert-butylphenoxyl radical. The reaction between LCuNO(2) and 2,4-di-tert-butylphenol was more complicated. It yielded two products: the coupled bisphenol product expected from a H-atom abstraction and 2,4-di-tert-butyl-6-nitrophenol, the product of an unusual anaerobic nitration. Various mechanisms for the latter transformation were considered.

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