CO2 methanation over Ni-promoted mesostructured silica nanoparticles: Influence of Ni loading and water vapor on activity and response surface methodology studies

被引:150
作者
Aziz, M. A. A. [1 ]
Jalil, A. A. [1 ,2 ]
Triwahyono, S. [3 ]
Saad, M. W. A. [2 ]
机构
[1] Univ Teknol Malaysia, Inst Hydrogen Econ, Utm Johor Bahru 81310, Johor, Malaysia
[2] Univ Teknol Malaysia, Fac Chem Engn, Dept Chem Engn, Utm Johor Bahru 81310, Johor, Malaysia
[3] Univ Teknol Malaysia, Fac Sci, Dept Chem, Utm Johor Bahru 81310, Johor, Malaysia
关键词
CO2; methanation; Ni/MSN; Basic sites; Water vapor; Response surface methodology (RSM); NATURAL-GAS; CATALYSTS; TEMPERATURE; ADSORPTION; STABILITY; HYDROGEN; PYRROLE; NICKEL; MCM-41;
D O I
10.1016/j.cej.2014.09.031
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The effects of Ni loading and water vapor on the properties of Ni/mesoporous silica nanoparticles (MSN) and CO2 methanation were studied. X-ray diffraction, N-2 adsorption-desorption, and pyrrole-adsorbed infrared (IR) spectroscopy results indicated that the increasing Ni loading (1-10 wt.%) decreased the crystallinity, surface area, and basic sites of the catalysts. The activity of CO2 methanation followed the order of 10Ni/MSN approximate to 5Ni/MSN > 3Ni/MSN > 1Ni/MSN. These results showed that the balance between Ni and the basic-site concentration is vital for the high activity of CO2 methanation. All Ni/MSN catalysts exhibited a high stability at 623 K for more than 100 h. The presence of water vapor in the feed stream induced a negative effect on the activity of CO2 methanation. The water vapor decreased the carbonyl species concentration on the surface of Ni/MSN, as evidenced by CO + H2O-adsorbed IR spectroscopy. The response surface methodology experiments were designed with face-centered central composite design (FCCCD) by applying 24 factorial points, 8 axial points, and 2 replicates, with one response variable (CO2 conversion). The Pareto chart indicated that the reaction temperature had the largest effect for all responses. The optimum CO2 conversion was predicted from the response surface analysis as 85% at an operating treatment time of 6 h, reaction temperature of 614 K, gas hourly space velocity (GHSV) of 69105 mL g(cat)(-1) and H-2/CO2 ratio of 3.68. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:757 / 764
页数:8
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