C-H bond activation of propane on Ga_(2)O_(2)^(2+)in Ga/H-ZSM-5 and its mechanistic implications

作     者：Zhaoqi Zhao Yunzhu Zhong Xiaoxia Chang Bingjun Xu 赵兆麒;钟云竹;常晓侠;徐冰君

作者机构：Beijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2024年第64卷第9期

页      面：32-43页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 0817[工学-化学工程与技术] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0703[理学-化学] 

基　　金：国家自然科学基金(22172001) 北京国家分子科学实验室资助 

主　　题：Propane dehydrogenation Ga2O22+ Activation of C-H bond Ga species 

摘      要：Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains ***_(2)O_(2)^(2+)stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent *** we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+)species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+)species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al *** disparity in Ga_(2)O_(2)^(2+)species stems from their differing capacity in completing the catalytic *** results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+)species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+)species corresponding to GaHHW.