Controllable synthesis of core-shell Co@C@SiO2 catalysts for enhancing product selectivity in Fischer-Tropsch synthesis by tuning the mass transfer resistance

被引:27
作者
Chen, Yao [1 ]
Li, Xin [1 ]
Dai, Liya [1 ]
Nisa, Mehar U. [1 ]
Liu, Chengchao [2 ,3 ]
Lv, Shuai [2 ,3 ]
Lv, Jing [1 ]
Li, Zhenhua [1 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Sch Chem Engn & Technol, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China
[2] South Cent Univ Nationalities, Key Lab Catalysis & Mat Sci State Ethn Affairs Co, Coll Chem & Mat Sci, Wuhan 430074, Hubei, Peoples R China
[3] South Cent Univ Nationalities, Minist Educ, Wuhan 430074, Hubei, Peoples R China
来源
JOURNAL OF ENERGY CHEMISTRY | 2020年 / 51卷
基金
中国国家自然科学基金;
关键词
Fischer-Tropsch synthesis; ZIF-67; Product selectivity; Core-shell catalyst; Hydrophilic property; METAL-ORGANIC FRAMEWORKS; DOPED CARBON NANOTUBES; WATER; REDUCTION; EFFICIENT; ZIF-67; COMPOSITES; PRECURSOR;
D O I
10.1016/j.jechem.2020.03.074
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Fischer-Tropsch synthesis (FTS) is the key step in converting syngas into clean fuels. Traditional supported catalysts for FTS are problematic because the active metal crystalline size is positively related to metal loading. Therefore, increasing active metal loading may reduce the cobalt time yield (CTY) since a high CTY is usually obtained when the Co size is 8 nm. Here, a ZIF-67 (Zeolitic imidazolate framework-67) with a MOF (Metal organic framework) structure is used as a precursor to prepare the Co@C catalyst with not only high cobalt loading (55.6 wt%) but also with a small cobalt crystal size (as small as 8.6 nm). Core shell Co@C@SiO2-X catalysts with different SiO2 shell thicknesses were successfully prepared by coating different amounts of TEOS on the outer surface of Co@C to modify product selectivity. Compared with 40 wt% Co/SiO2 catalyst, core-shell Co@C@SiO2-X catalysts exhibited improved FTS performance. Furthermore, different gaseous hourly space velocities (GHSVs) were used to obtain CO conversion at similar levels to compare CTY and the turnover frequency (TOF). Among the catalysts, the Co@C@SiO2-1 catalyst, with its better mass transfer ability and suitable hydrophilic property, presented the highest TOF (9.75 x 10(-3) s(-1)) and lowest CH4 selectivity (9.75%). In addition, heavy hydrocarbons were effectively suppressed with the increase in shell thickness due to the increased mass transfer resistance. (c) 2020 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
引用
收藏
页码:199 / 206
页数:8
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