Dynamic confinement catalysis in Fe-based CO2 hydrogenation to light olefins

被引:38
|
作者
Wang, Linkai [1 ,2 ]
Han, Yu [1 ]
Wei, Jian [1 ]
Ge, Qingjie [1 ]
Lu, Shijian [3 ,4 ]
Mao, Yanpeng [5 ]
Sun, Jian [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] China Univ Min & Technol, Jiangsu Key Lab Coal based Greenhouse Gas Control, Xuzhou 221008, Jiangsu, Peoples R China
[4] China Univ Min & Technol, Carbon Neutral Inst, Xuzhou 221008, Jiangsu, Peoples R China
[5] Shandong Univ, Sch Energy & Power Engn, Natl Engn Lab Reducing Emiss Coal Combust, Shandong Key Lab Energy Carbon Reduct & Resource U, Jinan 250061, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; hydrogenation; Light olefin; MOR; Diffusion; Dynamic confinement; FISCHER-TROPSCH SYNTHESIS; CARBON-DIOXIDE; SELECTIVE CONVERSION; STEAM CRACKING; ENERGY USE; ZEOLITE; CARBONYLATION; PROPYLENE; ETHYLENE; LIFETIME;
D O I
10.1016/j.apcatb.2023.122506
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Hydrogenation of CO2 into light olefins is an important route to carbon neutrality. Most of traditional researches focus on the catalyst component, structure, and promoter to enhance the selectivity of light olefins while ignoring the diffusion of products. Here, we report a NaFeZr-MOR composite catalyst for light olefin synthesis in CO2 hydrogenation via pore confinement. The selectivity in hydrocarbons and STY (Space-time yields) of C-2-4(=) is gradually increasing maximum up to 51.3% and 12.2 (mmol center dot g(cat)(-1 center dot)h(-1)), which lie in a high level among reported Fe-based catalysts. Further characterization revealed that the essence of selectivity change period is the accumulation and evolution of carbonaceous species, which causes the change of product diffusion behavior. It suppresses the escape of heavy hydrocarbons from MOR pores, leading to an increased light olefin, especially ethylene, which is called "dynamic confinement". These findings provide a new insight for controlling low-carbon product selectivity in CO2 hydrogenation.
引用
收藏
页数:10
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