Coutard Nathan, Goldberg Jonathan M, Valle Henry U, Cao Yuan, Jia Xiaofan, Jeffrey Philip D, Gunnoe T Brent, Groves John T
Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904, United States.
Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States.
Inorg Chem. 2022 Jan 17;61(2):759-766. doi: 10.1021/acs.inorgchem.1c03086. Epub 2021 Dec 28.
Photodriven oxidations of alkanes in trifluoroacetic acid using commercial and synthesized Fe(III) sources as catalyst precursors and dioxygen (O) as the terminal oxidant are reported. The reactions produce alkyl esters and occur at ambient temperature in the presence of air, and catalytic turnover is observed for the oxidation of methane in a pure O atmosphere. Under optimized conditions, approximately 17% conversion of methane to methyl trifluoroacetate at more than 50% selectivity is observed. It is demonstrated that methyl trifluoroacetate is stable under catalytic conditions, and thus overoxidized products are not formed through secondary oxidation of methyl trifluoroacetate.
报道了使用市售和合成的铁（III）源作为催化剂前体以及氧气（O₂）作为终端氧化剂，在三氟乙酸中光驱动的烷烃氧化反应。该反应生成烷基酯，在空气中于室温下发生，并且在纯O₂气氛中观察到了甲烷氧化的催化周转。在优化条件下，观察到甲烷转化为三氟乙酸甲酯的转化率约为17%，选择性超过50%。结果表明，三氟乙酸甲酯在催化条件下是稳定的，因此不会通过三氟乙酸甲酯的二次氧化形成过度氧化产物。
