Hydrogenation of CO2 to Light Olefins over ZnZrOx/SSZ-13

被引:49
作者
Chen, Siyu [1 ,2 ]
Wang, Jiachen [3 ]
Feng, Zhendong [1 ,2 ]
Jiang, Yiming [1 ,2 ]
Hu, Hanwen [1 ,4 ]
Qu, Yuanzhi [1 ,2 ]
Tang, Shan [1 ,2 ]
Li, Zelong [5 ]
Liu, Jiaxu [3 ]
Wang, Jijie [1 ]
Li, Can [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 101408, Peoples R China
[3] Dalian Univ Technol, Dept Catalyt Chem & Engn, State Key Lab Fine Chem, Dalian 116012, Liaoning, Peoples R China
[4] Xiamen Univ, Collaborat Innovat Ctr Chem Energy Mat, Coll Chem & Chem Engn, Xiamen 361005, Fujian, Peoples R China
[5] Lanzhou Univ, Coll Chem & Chem Engn, State Key Lab Appl Organ Chem, Key Lab Adv Catalysis Gansu Prov, Lanzhou 730000, Gansu, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; Hydrogenation; Light Olefins; SSZ-13; Tandem Catalysis; ZnZrOx; CATALYTIC PERFORMANCE; SELECTIVE CONVERSION; ACIDIC ZEOLITES; CARBON-DIOXIDE; MAS NMR; METHANOL; SAPO-34; HSAPO-34; SSZ-13; OXIDE;
D O I
10.1002/anie.202316874
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Converting CO2 to olefins is an ideal route to achieve carbon neutrality. However, selective hydrogenation to light olefins, especially single-component olefin, while reducing CH4 formation remains a great challenge. Herein, we developed ZnZrOx/SSZ-13 tandem catalyst for the highly selective hydrogenation of CO2 to light olefins. This catalyst shows C-2(=)-C-4(=) and propylene selectivity up to 89.4 % and 52 %, respectively, while CH4 is suppressed down to 2 %, and there is no obvious deactivation. It is demonstrated that the isolated moderate Bronsted acid sites (BAS) of SSZ-13 promotes the rapid conversion of intermediate species derived from ZnZrOx, thereby enhancing the kinetic coupling of the reactions and inhibit the formation of alkanes and improve the light olefins selectivity. Besides, the weaker BAS of SSZ-13 promote the conversion of intermediates into aromatics with 4-6 methyl groups, which is conducive to the aromatics cycle. Accordingly, more propene can be obtained by elevating the Si/Al ratio of SSZ-13. This provides an efficient strategy for CO2 hydrogenation to light olefins with high selectivity.
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页数:7
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