1, 3-Butadienen Hydrogenation on Supported Pd-Sn Bimetallic Catalysts Investigated by Parahydrogen-induced Polarization

doi:10.11938/cjmr20212952

Abstract

Abstract:

The selective hydrogenation of 1, 3-butadiene over Pd-Sn/Al₂O₃ bimetallic catalysts was investigated by heterogeneous parahydrogen-induced polarization (PHIP). A series of Pd₁-Sn_x/Al₂O₃ bimetallic catalysts with different Pd/Sn ratios were synthesized by incipient wetness co-impregnation method. It was observed that the Pd/Sn ratios of the catalysts had a significant effect on the reaction activity of 1, 3-butadiene and the selectivity to butene. A monotonic decrease of reaction conversion was observed as the Pd/Sn ratio decreased, while the selectivity to butene showed an opposite trend. This can be attributed to the ensemble effect and the ligand effect caused by the increasing tin component content: as the Pd/Sn ratio decreases, less palladium component was exposed on the surface, leading to low activity. The electronic properties of the Pd atoms were altered, which led to a weaker adsorption strength of the semi-hydrogenation product butene and an increased selectivity. Smaller Pd ensembles were exposed on Sn-rich catalysts surface, which favored a higher ratio of pairwise addition process, leading to a stronger PHIP effect. The isomerization measurements by PASADENA (parahydrogen and synthesis allow for dramatically enhanced nuclear alignment) showed that the isomerization process between 1-butene and 2-butene decreased with the increase of Sn content. This can be accounted for by the easier desorption of 1-butene on Sn-rich catalysts.

Key words: 1,3-butadiene hydrogenation, bimetallic catalyst, nuclear magnetic resonance (NMR), isomerization process, parahydrogen-induced polarization (PHIP)

CLC Number:

O482.53

Han HU,Wei-yu WANG,Jun XU,Feng DENG. 1, 3-Butadienen Hydrogenation on Supported Pd-Sn Bimetallic Catalysts Investigated by Parahydrogen-induced Polarization[J]. Chinese Journal of Magnetic Resonance, 2022, 39(2): 133-143.

Figures/Tables 7

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