American Chemical Society
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Effect of H2 Preadsorption on CO Interactions with a Co/Re/Zr/SiO2‑Based Catalyst: In Situ DRIFTS Study

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journal contribution
posted on 2019-02-11, 00:00 authored by Nitin Kumar, George G. Stanley, J. J. Spivey
The effect of H2 preadsorption on the adsorption of CO on a 10% Co, 4% Re/(2% Zr/SiO2) catalyst was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) at different temperatures. CO adsorption experiments were carried out on a bare catalytic surface (reduced in flowing hydrogen, followed by flush with helium) and on the surface preadsorbed with H2. Results at room temperature showed less linearly adsorbed CO on the H2-preadsorbed surface than the bare surface. On a bare surface at room temperature, CO adsorbed producing a broad band covering a wide range of wavenumbers. CO adsorption over a H2-preadsorbed surface, in marked contrast, generated a narrower band, representing a more uniform set of Co–CO coordination sites. This indicates that H2 precoordination at room temperature blocks a number of different cobalt coordination sites, which allows CO coordination to a more electronically uniform set of cobalt sites. The results at temperatures from 230 to 300 °C, however, were found to be opposite, that is, much more adsorbed CO was found over a H2-preadsorbed surface than the bare surface, suggesting that the catalyst surface is modified by H2 at higher temperatures and facilitates CO adsorption. Syngas (1:1 H2/CO) flow over bare and H2-preadsorbed surfaces resulted in intermediate peak intensities compared to CO adsorption over either a bare surface or H2-preadsorbed cobalt surface.