4.8 Article

Breaking the inverse relationship between catalytic activity and selectivity in acetylene partial hydrogenation using dynamic metal-polymer interaction

期刊

JOURNAL OF CATALYSIS
卷 404, 期 -, 页码 716-725

出版社

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.09.017

关键词

Partial hydrogenation; Acetylene; Dynamic metal-polymer interaction; Palladium; Polyphenylene sulfide

资金

  1. Basic Science Research Program through the National Research Foundation of Korea [NRF-2020R1A2C3003694]
  2. Institute for Basic Science [IBS-R004]
  3. LG Chem

向作者/读者索取更多资源

By introducing Am-PPS as a promoter, modifying the catalyst led to a significant enhancement of ethylene selectivity and acetylene hydrogenation activity, possibly due to the selective adsorption of acetylene and H-2 at the Am-PPS-Pd interface. The modified catalyst showed excellent long-term stability, demonstrating the unique potential of dynamic metal-polymer interaction in designing partial hydrogenation catalysts.
The partial hydrogenation of acetylene impurities in ethylene is industrially important because acetylene acts as a catalyst poison in downstream ethylene polymerization processes. In this reaction, simultaneously achieving high acetylene conversion and partial hydrogenation selectivity is challenging, and most known catalyst systems exhibit an inverse activity-selectivity relationship. Here, an amorphous polyphenylene sulfide (Am-PPS) was synthesized as a promoter for 0.1 wt% Pd/alpha-Al2O3. The catalyst modification using a trace amount of Am-PPS (0.15 wt%) enabled a remarkable enhancement of ethylene selectivity without an appreciable loss in acetylene hydrogenation activity. This could be attributed to the dynamic change of the Am-PPS-Pd interface, which selectively allows the cooperative adsorption of acetylene and H-2, but not ethylene. Besides, the modified catalyst exhibited excellent long-term stability because of the high thermochemical stability of the polymer. These results demonstrate the unique possibility of using dynamic metal-polymer interaction to design partial hydrogenation catalysts that simultaneously exhibit high activity, selectivity, and stability. (C) 2021 Elsevier Inc. All rights reserved.

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