CO2 hydrogenation to light olefins with high-performance Fe0.30Co0.15Zr0.45K0.10O1.63

被引:48
作者
Ding, Jie [1 ,2 ,3 ]
Huang, Liang [4 ]
Gong, Weibo [2 ,3 ]
Fan, Maohong [2 ,3 ,5 ]
Zhong, Qin [1 ]
Russell, Armistead G. [5 ]
Gu, Hao [1 ]
Zhang, Haijun [4 ]
Zhang, Yulong [6 ]
Ye, Run-ping [2 ,3 ]
机构
[1] Nanjing Univ Sci & Technol, Sch Chem Engn, Nanjing 210094, Jiangsu, Peoples R China
[2] Univ Wyoming, Dept Chem, Laramie, WY 82071 USA
[3] Univ Wyoming, Dept Petr Engn, Laramie, WY 82071 USA
[4] Wuhan Univ Sci & Technol, State Key Lab Refractories & Met, Wuhan 430081, Hubei, Peoples R China
[5] Georgia Inst Technol, Sch Civil & Environm Engn, Atlanta, GA 30332 USA
[6] Henan Polytech Univ, Coll Chem & Chem Engn, Jiaozuo 454000, Henan, Peoples R China
基金
中国国家自然科学基金;
关键词
Catalytic CO(2 )hydrogenation; Iron based catalysts; Oxygen vacancies; Surface hydroxyl sites; Ethylene synthesis; FISCHER-TROPSCH SYNTHESIS; METAL-ORGANIC FRAMEWORKS; HIGH-SURFACE-AREA; OXYGEN VACANCIES; CARBON-DIOXIDE; CATALYTIC PERFORMANCE; SELECTIVE CONVERSION; METHANOL SYNTHESIS; TEMPORAL ANALYSIS; LATTICE OXYGEN;
D O I
10.1016/j.jcat.2019.07.036
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
The study was designed to investigate the catalytic hydrogenation of increasingly concerned CO2 to light olefins including ethylene, propylene and butylene, a series of critically important materials for various chemical syntheses, a win-win scenario for environment and economy. The Fe0.30Co0.15Zr0.30K0.10O1.63 catalyst, presented much poorer surface hydroxyl groups but richer oxygen vacancies (OVs) than the Fe0.60Co0.30K0.10O1.40, displayed light olefin space time yields (STY) of 4.93 mmol.g(cat)(-1).h(-1) at 310 degrees C and 2.0 MPa, which was 33.24% higher than the Fe0.60Co0.30K0.10O1.40 at the same reaction conditions. Extensive characterizations demonstrate that both oxygen vacancies (OVs) and surface hydroxyl groups (-OH) played important roles in the catalytic CO2 hydrogenation to light olefins, while OVs were more critical. OVs on the reduced Fe0.30Co0.15Zr0.45K0.10O1.63 were more active than those on the reduced Fe0.60Co0.30K0.10O1.40, which was very important to the enhancement of the oxygen storage, adsorption and activation of CO2 and thus the direct and efficient conversion of CO2 into CO, an important intermediate for the synthesis of light olefins synthesis. Thus, Fe0.30Co0.15Zr0.30K0.10O1.63 is a promising catalyst for converting CO2 hydrogenation to light olefins. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:224 / 232
页数:9
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