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Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane
Chem ( IF 19.1 ) Pub Date : 2020-08-12 , DOI: 10.1016/j.chempr.2020.07.011
Zhenhua Xie , Dong Tian , Meng Xie , Shi-Ze Yang , Yuanguo Xu , Ning Rui , Ji Hoon Lee , Sanjaya D. Senanayake , Kongzhai Li , Hua Wang , Shyam Kattel , Jingguang G. Chen

Selective upgrading of underutilized ethane in shale gas with greenhouse gas CO2 can produce syngas via dry reforming (C–C bond scission) or ethylene via oxidative dehydrogenation (C–H bond scission). However, it remains challenging to identify active sites responsible for the selective bond cleavage in ethane due to the complexity of supported catalysts. Herein, the ethane-CO2 reaction over CeO2-supported catalysts was investigated to unravel the functions of distinct interfacial sites by combining kinetic measurements with in situ characterizations and calculations: the Pd/CeOx interface is responsible for supplying reactive oxygen species, electron-deficient oxygen species on Pd surface boosts the non-selective bond scission to produce syngas, electron-enriched oxygen in the FeOx/Pd interface enhances the selective scission of C–H bond to yield ethylene, and the FeOx/CeO2 interaction mediates oxygen supply and confines metal ensembles. The current work identifies opportunities for using different interfacial structures in upgrading abundant shale gas and CO2.



中文翻译:

乙烷中CO 2辅助选择性裂解C–C / C–H键的界面活性位点

页岩气中未充分利用的乙烷与温室气体CO 2的选择性提质可以通过干重整(CC键断裂)产生合成气,或通过氧化脱氢(CH键断裂)产生乙烯。然而,由于负载的催化剂的复杂性,鉴定负责乙烷中的选择性键裂解的活性位点仍然具有挑战性。本文中,通过结合动力学测量与原位表征和计算,研究了CeO 2负载的催化剂上的乙烷-CO 2反应,以揭示不同界面部位的功能:Pd / CeO x界面负责提供活性氧,Pd表面缺电子的氧会促进非选择性键断裂,产生合成气,FeO x / Pd界面中的电子富集氧会增强C–H键的选择性断裂,从而产生乙烯和FeO x / CeO 2相互作用介导氧气供应并限制金属团簇。当前的工作确定了使用不同界面结构提升页岩气和CO 2丰富度的机会。

更新日期:2020-10-08
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