Slurry phase methanation of carbon monoxide over nanosized Ni-Al2O3 catalysts prepared by microwave-assisted solution combustion

被引:31
作者
Gao, Yuan [1 ]
Meng, Fanhui [1 ]
Ji, Keming [1 ]
Song, Yan [1 ]
Li, Zhong [1 ]
机构
[1] Taiyuan Univ Technol, Inst Coal Chem Engn, Minist Educ & Shanxi Prov, Key Lab Coal Sci & Technol, Taiyuan 030024, Shanxi, Peoples R China
基金
中国博士后科学基金;
关键词
Slurry-bed reactor; CO methanation; Synthetic natural gas; Ni-Al2O3; catalyst; Microwave-assisted solution combustion; FISCHER-TROPSCH SYNTHESIS; NI/AL2O3; CATALYSTS; CO METHANATION; NATURAL-GAS; HYDROGEN-PRODUCTION; TOTAL OXIDATION; H-2-RICH GAS; FIXED-BED; PERFORMANCE; SYNGAS;
D O I
10.1016/j.apcata.2015.11.006
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 clean transformation of coal into natural gas is an interesting topic in green chemistry, as well as a promising process for the production of natural gas. In the present work, the methanation of CO was performed in a slurry-bed reactor with a series of nanosized Ni-Al2O3 catalysts prepared by microwave assisted solution combustion with different fuels (urea, glycine, ethylene glycol and citric acid). As compared with other fuels, a majority of urea and nitrates simultaneously decompose and occur in extensive overlapped temperature ranges during heating, which is conducive to the formation of a moderate and sustained combustion reaction. In addition, the thermodynamic calculation and thermogravimetric analysis indicate that the amount of heat generated during combustion is the minimum when urea was used as fuel. By the formation of a stable combustion and a relative low combustion temperature, the NiAl-U catalyst exhibits the largest BET area and metal surface area, the smallest Ni particle size and more dispersive Ni species, as evidenced by XRD, TEM, N-2 adsorption-desorption, H-2-TPR and H-2 pulse chemisorption characterizations. In the slurry methanation of CO, the conversion of CO and selectivity for CH4 over NiAl-U catalyst reach up to 95.7% and 96.2% at 300 degrees C, 1.0 MPa and 3000 mL/g(cat) h, respectively, which are superior to those of other combustion-synthesized catalysts and commercial catalyst. In addition, The NiAl-U catalyst exhibits significant improvement in anti-sintering during 200 h lifetime test, mainly because of smaller Ni particle size, high dispersity of Ni active species on support and high stability of support. The findings presented here are expected to provide new approaches for rational design of nanosized Ni-Al2O3 catalysts for CO methanation reactions in slurry phase. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:74 / 83
页数:10
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