Alcohol Synthesis from CO2 , H2 , and Olefins over Alkali-Promoted Au Catalysts-A Catalytic and In situ FTIR Spectroscopic Study

ChemSusChem. 2019 Feb 7;12(3):651-660. doi: 10.1002/cssc.201801937. Epub 2018 Dec 14.

Abstract

Au/TiO2 and Au/SiO2 catalysts containing 2 wt % Au and different amounts of K or Cs were tested for alcohol synthesis from CO2 , H2 , and C2 H4 /C3 H6 . 1-Propanol or 1-butanol/isobutanol were obtained in the presence of C2 H4 or C3 H6 . Higher yields of the corresponding alcohols were obtained over TiO2 -based catalysts in comparison with their SiO2 -based counterparts. This is caused by an enhanced ability of the TiO2 -based catalysts for CO2 activation, as concluded from in situ fourier-transform infrared (FTIR) spectroscopy and temporal analysis of products (TAP) studies. The synthesized carbonate and formate species adsorbed on the support do not hamper CO2 conversion into CO and the hydroformylation reaction. The transformation of Auδ+ to active Au0 sites proceeds during an activation procedure. As reflected by CO adsorption and scanning transmission electron microscopy, the accessible Au0 sites are influenced by the amount of alkali dopants and the support. FTIR data and TAP tests reveal a very weak interaction of C2 H4 with the catalyst, suggesting its quick reaction with CO and H2 after activation on Au0 sites to form propanol and propane.

Keywords: Au nanoparticles; alcohol synthesis; carbon dioxide conversion; heterogeneous catalysis; in situ FTIR spectroscopy.