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Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis

Abstract

Gas-phase hydrogenation of 1,3-butadiene was investigated over Pt/SiO2 catalyst with the aim to understand the complete hydrogenation of diene. The measurements focused on the effect of Pt dispersion on the product distribution and the kinetics of n-butane formation. Under the investigated conditions with an excess of hydrogen, the selectivity to n-butane sharply decreased from 41.6% to less than 3% at 1,3-butadiene conversion of ~10% when the average Pt particle size increased from 3.9 to 22 nm. Correspondingly, the apparent activation energy for n-butane formation was measured to be increased by about 2.7 times. In situ diffuse reflectance infrared fourier transform (DRIFT) observations via alternating 1,3-butadiene and hydrogen feeds over the catalysts demonstrated that 1-butene was the major reaction intermediate in the process of 1,3-butadiene hydrogenation. By analysis of the kinetic data using the Horiuti-Polanyi mechanism with 1-butene as the intermediate, different reactivities of hydrogen on the catalysts towards C=C bond hydrogenation were proposed to understand the variation of the selectivity to n-butane with Pt dispersion. This viewpoint was further supported by DFT calculation of 1-butene hydrogenation with hydrogen at different sites on Pt(111) surface.

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Publication details

The article was received on 20 Mar 2017, accepted on 10 May 2017 and first published on 11 May 2017


Article type: Paper
DOI: 10.1039/C7CY00534B
Citation: Catal. Sci. Technol., 2017, Accepted Manuscript
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    Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis

    C. Hu, J. Sun, D. Kang, Q. Zhu and Y. Yang, Catal. Sci. Technol., 2017, Accepted Manuscript , DOI: 10.1039/C7CY00534B

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