期刊
ACS CATALYSIS
卷 10, 期 15, 页码 8515-8523出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c02452
关键词
carbon deposition; strong metal-support interaction; gold catalysis; FTIR; EELS; CO oxidation
资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program
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 degrees 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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