Aerobic Electrochemical Oxygenation of Light Hydrocarbons Catalyzed by an Iron-Tungsten Oxide Molecular Capsule

Marco Bugnola, Raanan Carmieli, Ronny Neumann

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

The selective oxidation of light hydrocarbons and their valorization with only dioxygen (O2) 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 O2 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 O2 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.

Original languageEnglish
Pages (from-to)3232-3236
Number of pages5
JournalACS Catalysis
Volume8
Issue number4
DOIs
Publication statusPublished - Apr 6 2018

Fingerprint

Oxygenation
Hydrocarbons
Capsules
Tungsten
Iron
Oxidation
Oxides
Carbon
Hydroxylation
Alkanes
Ethane
Ozone
Alkenes
Mixed Function Oxygenases
Oxidants
Acetic acid
Acetic Acid
Paraffins
Sulfates
Olefins

Keywords

  • C-H bond activation
  • cathodic oxidation
  • electrocatalysis
  • hydroxylation
  • Polyoxometalate

ASJC Scopus subject areas

  • Catalysis

Cite this

Aerobic Electrochemical Oxygenation of Light Hydrocarbons Catalyzed by an Iron-Tungsten Oxide Molecular Capsule. / Bugnola, Marco; Carmieli, Raanan; Neumann, Ronny.

In: ACS Catalysis, Vol. 8, No. 4, 06.04.2018, p. 3232-3236.

Research output: Contribution to journalArticle

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