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Dynamic metal-polymer interaction for the design of chemoselective and long-lived hydrogenation catalysts.
Science Advances ( IF 11.7 ) Pub Date : 2020-07-08 , DOI: 10.1126/sciadv.abb7369
Songhyun Lee 1 , Seung-Jae Shin 2 , Hoyong Baek 1 , Yeonwoo Choi 1 , Kyunglim Hyun 1 , Myungeun Seo 2, 3 , Kyunam Kim 1 , Dong-Yeun Koh 1 , Hyungjun Kim 2 , Minkee Choi 1
Affiliation  

Metal catalysts are generally supported on hard inorganic materials because of their high thermochemical stabilities. Here, we support Pd catalysts on a thermochemically stable but “soft” engineering plastic, polyphenylene sulfide (PPS), for acetylene partial hydrogenation. Near the glass transition temperature (~353 K), the mobile PPS chains cover the entire surface of Pd particles via strong metal-polymer interactions. The Pd-PPS interface enables H2 activation only in the presence of acetylene that has a strong binding affinity to Pd and thus can disturb the Pd-PPS interface. Once acetylene is hydrogenated to weakly binding ethylene, re-adsorption of PPS on the Pd surface repels ethylene before it is further hydrogenated to ethane. The Pd-PPS interaction enables selective partial hydrogenation of acetylene to ethylene even in an ethylene-rich stream and suppresses catalyst deactivation due to coke formation. The results manifest the unique possibility of harnessing dynamic metal-polymer interaction for designing chemoselective and long-lived catalysts.



中文翻译:


用于设计化学选择性和长寿命加氢催化剂的动态金属-聚合物相互作用。



金属催化剂由于其高热化学稳定性而通常负载在硬质无机材料上。在这里,我们将钯催化剂负载在热化学稳定但“软”的工程塑料聚苯硫醚(PPS)上,用于乙炔部分氢化。在玻璃化转变温度(~353 K)附近,移动的 PPS 链通过强金属-聚合物相互作用覆盖 Pd 颗粒的整个表面。 Pd-PPS界面仅在存在乙炔的情况下才能够激活H 2 ,乙炔对Pd具有很强的结合亲和力,因此可以干扰Pd-PPS界面。一旦乙炔被氢化成弱结合乙烯,PPS 在 Pd 表面上的重新吸附就会排斥乙烯,然后再进一步氢化成乙烷。即使在富含乙烯的物流中,Pd-PPS 相互作用也能够将乙炔选择性部分加氢为乙烯,并抑制由于焦炭形成而导致的催化剂失活。结果表明,利用动态金属-聚合物相互作用来设计化学选择性和长寿命催化剂的独特可能性。

更新日期:2020-07-08
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