期刊
MICROPOROUS AND MESOPOROUS MATERIALS
卷 187, 期 -, 页码 125-134出版社
ELSEVIER
DOI: 10.1016/j.micromeso.2013.12.023
关键词
APTES; Grafted silicas; CO2; Chemisorption; Pore expanding agents
类别
资金
- Spanish Ministry of Economy and Competitiveness [CTQ2012-37925-C03-03]
- FEDER
- Regional Government (Junta de Andalucia) [P09-FQM-5070]
- European Union [295156, FP7-PEOPLE-2011-IRSES]
- [PHB2011-0074-PC]
The CO2 adsorption capacity of different APTES-grafted mesoporous silicas of SBA-15 type has been investigated and the influence of support textural properties and the role of the presence of silanol groups on the adsorption capacity are analyzed. Four adsorbents based on SBA-15 were prepared using tetraethyl orthosilicate (TEOS) as silicon source, with and without the addition of trimethyl-benzene (TMB) and n-heptane as swelling agents, and adding in some cases ammonium fluoride as a solubility enhancer. 3-(triethoxysilyl)propylamine (APTES) was then used as grafting agent by reaction with free silanol groups on the silica surface so as to provide pending amino groups for CO2 capture. The adsorption behavior for all supports was adequately described by a Freundlich model, whereas for the APTES-grafted silica, a dual-site Langmuir model was applied, which allowed us to quantify and qualify two different adsorption sites. The addition of n-heptane as swelling agent led to pore sizes beyond 10 nm and improved significantly the grafting efficiency, leading to higher CO2 uptakes as compared to the starting supports. At 1 bar and 25 degrees C and anhydrous conditions, CO2 uptakes of 2.4 mmol g(-1) or 0.64 mol CO2 per mol N were achieved (which reveals a significant contribution of physisorption). This sample could be successfully regenerated at 100 degrees C, maintaining a constant capacity for 3 adsorption-desorption cycles. At 0.15 bar and 60 degrees C, anhydrous conditions, CO2 uptake reaches 1.5 mmol g(-1). This value may be theoretically doubled in the presence of humidity, and there is room for further improvement if supports with the same pore size (13 nm) and higher surface areas (e.g. 1000 m(2)/g) are successfully synthesized. (C) 2013 Elsevier Inc. All rights reserved.
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