Login / Signup

Selective Methane Oxidation by Heterogenized Iridium Catalysts.

Haoyi LiMuchun FeiJennifer L TroianoLu MaXingxu YanPeter TieuYucheng YuanYuhan ZhangTianying LiuXiaoqing PanGary W BrudvigDunwei Wang
Published in: Journal of the American Chemical Society (2023)
Oxidative methane (CH 4 ) carbonylation promises a direct route to the synthesis of value-added oxygenates such as acetic acid (CH 3 COOH). Here, we report a strategy to realize oxidative CH 4 carbonylation through immobilized Ir complexes on an oxide support. Our immobilization approach not only enables direct CH 4 activation but also allows for easy separation and reutilization of the catalyst. Furthermore, we show that a key step, methyl migration, that forms a C-C bond, is sensitive to the electrophilicity of carbonyl, which can be tuned by a gentle reduction to the Ir centers. While the as-prepared catalyst that mainly featured Ir(IV) preferred CH 3 COOH production, a reduced catalyst featuring predominantly Ir(III) led to a significant increase of CH 3 OH production at the expense of the reduced yield of CH 3 COOH.
Keyphrases
  • room temperature
  • ionic liquid
  • highly efficient
  • carbon dioxide
  • metal organic framework
  • reduced graphene oxide
  • mass spectrometry
  • liquid chromatography
  • magnetic nanoparticles