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Breaking the inverse relationship between catalytic activity and selectivity in acetylene partial hydrogenation using dynamic metal–polymer interaction
Journal of Catalysis ( IF 6.5 ) Pub Date : 2021-09-22 , DOI: 10.1016/j.jcat.2021.09.017
Younghwan Park 1 , Songhyun Lee 1 , Kyunglim Hyun 1 , Jueun Lee 1 , Jeong Young Park 2, 3 , Ryong Ryoo 2, 3 , Minkee Choi 1, 3
Affiliation  

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/α-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 H2, 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.



中文翻译:

利用动态金属-聚合物相互作用打破乙炔部分加氢催化活性和选择性之间的反比关系

乙烯中乙炔杂质的部分加氢在工业上很重要,因为乙炔在下游乙烯聚合过程中充当催化剂毒物。在该反应中,同时实现高乙炔转化率和部分加氢选择性具有挑战性,并且大多数已知的催化剂体系表现出逆活性-选择性关系。在此,合成了无定形聚苯硫醚 ( Am -PPS) 作为 0.1 wt% Pd/ α -Al 2 O 3的促进剂。使用微量Am的催化剂改性-PPS (0.15 wt%) 能够显着提高乙烯选择性,而乙炔加氢活性没有明显损失。这可能归因于Am -PPS-Pd 界面的动态变化,它选择性地允许乙炔和 H 2的协同吸附,而不是乙烯。此外,由于聚合物的高热化学稳定性,改性催化剂表现出优异的长期稳定性。这些结果证明了使用动态金属-聚合物相互作用来设计同时具有高活性、选择性和稳定性的部分氢化催化剂的独特可能性。

更新日期:2021-09-23
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