Alcohol-Induced Low-Temperature Blockage of Supported-Metal
Catalysts for Enhanced Catalysis
Posted on 2020-07-20 - 14:05
The
partial or complete blockage of active sites of metal nanoparticles
(NPs) on supported-metal catalysts has been of interest for tuning
the stability, selectivity, and rate of reactions. Here, we show that
Au-sites in Au/TiO2 surprisingly become blocked upon treatment
in common alcohols (2-propanol and methanol), with 2-propanol causing
a greater extent of blockage. Nearly 95% of Au-sites are covered after
treatment in 2-propanol at room temperature, followed by desorption
at 150 °C. Infrared spectroscopy of CO adsorption unambiguously
confirms the occurrence of this phenomenon. Electron energy loss spectroscopy
(EELS), temperature-programmed desorption (TPD), Raman spectroscopy,
and DFT simulations suggest that the formation of carbon deposits
from 2-propanol decomposition and/or the migration of a TiOx layer over the supported NPs may be responsible
for the blockage of Au-sites. Nearly full coverage of Au NPs after
treatment in 2-propanol led to negligible activity for catalytic CO
oxidation, whereas partial retraction of the overlayer led to enhanced
activity with time-on-stream, suggesting a self-activating catalytic
performance.
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Polo-Garzon, Felipe; Blum, Thomas F.; Fung, Victor; Bao, Zhenghong; Chen, Hao; Huang, Zhennan; et al. (2020). Alcohol-Induced Low-Temperature Blockage of Supported-Metal
Catalysts for Enhanced Catalysis. ACS Publications. Collection. https://doi.org/10.1021/acscatal.0c02452