Bifunctional Catalysts with Separated and Tunable Sites on Zeolites for Relay Catalysis of the Oxidative Dehydrogenation of Propane Using CO2

被引:0
|
作者
Li, Wanting [1 ,2 ]
Wang, Tianchang [1 ]
Cao, Xinxin [1 ,2 ]
Li, Yuze [1 ,2 ]
Miao, Gai [1 ]
Sun, Nannan [1 ,2 ,3 ]
Li, Jiong [4 ]
Han, Wei [5 ]
Wei, Wei [1 ,2 ,3 ]
Chen, Xinqing [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Shanghai Adv Res Inst, State Key Lab Low Carbon Catalysis & Carbon Dioxid, Shanghai 201210, Peoples R China
[4] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[5] Hong Kong Univ Sci & Technol, Div Environm & Sustainabil, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
关键词
bifunctional catalysts; CO2; utilization; heterogeneous catalysis; propane dehydrogenation; zeolite; LIGHT ALKANES; REDUCTION; CERIA;
D O I
10.1002/adfm.202414231
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The oxidative dehydrogenation of propane using (CO2-ODH) technology has broad application prospects in the production of propylene and the utilization of CO2, and the development of efficient CO2-ODH catalysts is of great significance. However, it remains a challenge to develop a highly efficient catalyst that can activate both C & horbar;H and C & boxH;O. Herein, a PtZn/Co@S-1 catalyst with a very low precious metal content of 0.2 wt.% is reported. Benefiting from the PtZn4 nanoclusters dispersed on the surface of Silicalite-1 zeolite and tetrahedrally coordinated Co2+ in the Silicalite-1 zeolite framework via relay catalysis, the independent dual sites structure (PtZn/Co@S-1) greatly promotes CO2-ODH reaction with a high conversion rate of both C3H8 (59.7%) and CO2(44.3%), and propylene selectivity of 94.9%, thus upsetting the equilibrium for direct dehydrogenation of propane. Experimental measurements and density functional theory calculations suggest that the PtZn4 and Co2+ interfaces are likely propane dehydrogenation and carbon dioxide hydrogenation active sites respectively.
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页数:10
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