期刊
ACS CATALYSIS
卷 8, 期 4, 页码 3232-3236出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b00477
关键词
polyoxometalate; electrocatalysis; cathodic oxidation; C-H bond activation; hydroxylation
资金
- Israel Science Foundation [2046/14]
- Divadol Foundation
The selective oxidation of light hydrocarbons and their valorization with only dioxygen (O-2) are important transformations toward development of efficient chemical processes. Monooxygenase enzymes can catalyze selective aerobic reactions under reducing and protic conditions. The translation of such enzymatic pathways to the practical electrocatalytic oxidation of light, gaseous hydrocarbons, using O-2 as sole oxidant is now reported. An iron tungsten oxide inorganic molecular catalyst with a capsular structure {Fe30W72} stabilized inside by sulfate/bisulfate anions provides a protic environment where three iron atoms are located at each of the pores of the capsule leading to a unique and potent active site for the oxidation reactions. Under mild electrochemical conditions, 1.8 V, in water at room temperature, using O-2 from air, we demonstrate the low-pressure (1-2 bar) hydroxylation of alkanes, notably ethane to acetic acid, and the ozone like cleavage of the carbon carbon double bonds of alkenes. Typical turnover frequencies were 300-400 min(-1). Initial mechanistic studies support a reaction through a very active iron-oxo species.
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