Enhanced CH3OH selectivity in CO2 hydrogenation using Cu-based catalysts generated via SOMC from GaIII single-sites.

Chemical Science
Erwin LamChristophe Copéret

Abstract

Small and narrowly distributed nanoparticles of copper alloyed with gallium supported on silica containing residual GaIII sites can be obtained via surface organometallic chemistry in a two-step process: (i) formation of isolated GaIII surface sites on SiO2 and (ii) subsequent grafting of a CuI precursor, [Cu(O t Bu)]4, followed by a treatment under H2 to generate CuGa x alloys. This material is highly active and selective for CO2 hydrogenation to CH3OH. In situ X-ray absorption spectroscopy shows that gallium is oxidized under reaction conditions while copper remains as Cu0. This CuGa material only stabilizes methoxy surface species while no formate is detected according to ex situ infrared and solid-state nuclear magnetic resonance spectroscopy.

References

Apr 21, 2012·Science·Malte BehrensRobert Schlögl
Dec 5, 2012·Angewandte Chemie·George A Olah
Jun 18, 2014·Chemical Society Reviews·Alain GoeppertGeorge A Olah
May 21, 2016·Science·Sebastian KuldJens Sehested
Jun 18, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·James P DombrowskiT Don Tilley
Aug 30, 2016·Journal of the American Chemical Society·Shyam KattelPing Liu
Jul 22, 2018·Journal of the American Chemical Society·Erwin LamChristophe Copéret
Aug 28, 2018·Journal of the American Chemical Society·Keith SearlesChristophe Copéret

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Methods Mentioned

BETA
X-ray
nuclear magnetic resonance
NMR

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