The influences of template dodecylamine on CO2 adsorption to Amine-modified HMS
REN Jie1, LIU Feng-ling1, QIU Hui1, LU Xia1,2, LU Shuai-shuai1, GUO Zhao-bing1
1. Collaborative Innovation Center of Atmospheric Environment and Equipment Technologies, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China;
2. Hebi City Meteorological Bureau, Hebi 458000, China
The mesoporous silica HMS marked as HMS-1was prepared using tetraethyl orthosilicate as silica source and dodecylamine as template. Its template was removed by calcination and ethanol extraction. The materials without template was marked as HMS-2 (Calcined material) and HMS-3 (ethanol extraction). HMS-1, HMS-2 and HMS-3 were modified with mixed tetraethylenepentamine and diethanolamine. The structures of these materials were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) and N2 adsorption/desorption experiment. The adsorption properties and regeneration ability of the materials toward CO2 with low concentration at atmosphere pressure were studied. The results of XRD and FTIR showed that TEPA and DEA were loaded into the pores of HMS successfully. The N2 adsorption/desorption experiment showed that the pore volume of HMS-1 and modified HMS was significantly lower than that of HMS-2 and HMS-3. At 20oC, the adsorption amount of CO2 with initial concentration of 10% follows an order of MA-HMS-1 (3.29mmol/g) > MA-HMS-3 (2.7mmol/g) > HMS-1 (1.88mmol/g) > MA-HMS-2 (1.65mmol/g) > HMS-2 (1.33mmol/g), indicating that the template, diethanolamine, presented in HMS not only increases the adsorption sites, but also had synergistic effects on CO2 adsorption to HMS functionalized with the mixed organic amines too. As temperature ranged from 20oC to 75oC, MA-HMS-1 and MA-HMS-3 adsorption were affected obviously and its amount reached the maximum at 65oC. The adsorption amount of HMS-1 decreased consecutively with elevating temperature and MA-HMS-2 had almost a constant adsorption amount. The amine-containing materials, HMS-1, MA-HMS-1, MA-HMS-2 and MA-HMS-3, had excellent regeneration capability at 80oC. After four times of continuous adsorption-desorption cycles, the regenerating ratio of MA-HMS-1 (97.5%) was much higher than that of MA-HMS-2 (83%) and MA-HMS-3 (84%), reflecting that the preserved template improved the regeneration capacity obviously.
任杰, 刘凤玲, 邱慧, 卢霞, 陆帅帅, 郭照冰. 模板剂十二胺对胺改性HMS吸附CO2的影响[J]. 中国环境科学, 2018, 38(4): 1274-1279.
REN Jie, LIU Feng-ling, QIU Hui, LU Xia, LU Shuai-shuai, GUO Zhao-bing. The influences of template dodecylamine on CO2 adsorption to Amine-modified HMS. CHINA ENVIRONMENTAL SCIENCECE, 2018, 38(4): 1274-1279.
Ye Q, Jiang J Q, Wang C X, et al. Adsorption of low-concentration carbon dioxide on amine-modified carbon nanotubes at ambient temperature[J]. Energy & Fuels, 2012,26(4):2497-2504.
[3]
Nugent P, Belmabkhout Y, Burd S D, et al. Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation[J]. Nature, 2013,495(7439):80-84.
[4]
Qian D, Lei C, Wang E M, et al. A method for creating microporous carbon materials with excellent CO2-adsorption capacity and selectivity[J]. Chemsuschem, 2014,7(1):291-298.
Wei J W, Liao L, Xiao Y, et al. Capture of carbon dioxide by amine-impregnated as-synthesized MCM-41[J]. Journal of Environmental Sciences. 2010,22(10):1558-1563.
Yue M B, Chun Y, Cao Y, et al. CO2 capture by as-prepared SBA-15with an occluded organic template[J]. Advanced Functional Materials, 2006,16(13):1717-1722.
[12]
Yue M B, Sun L B, Cao Y, et al. Promoting the CO2adsorption in the amine-containing SBA-15by hydroxyl group[J]. Microporous and Mesoporous Materials, 2008,114:74-81.
[13]
Yu W H, Zhou C H, Ni Z M, et al.Enhancing isolated Ti (IV) framework sites in HMS[J]. Chemical Research in Chinese University, 23(2):127-130.
[14]
Zhao X S, Lu G Q, Whittaker A K, et al. Comprehensive Study of Surface Chemistry of MCM-41Using 29Si CP/MAS NMR, FTIR, Pyridine-TPD, and TGA[J]. Journal of Physical Chemistry B, 1997,101(33):6525-6531.
[15]
Wang W Z, Pauly T R, Pinnvaia T J. Tailoring the framework and textural mesopores of HMS molecular sieves through an electrically neutral (S°I°) assembly pathway[J]. Chemistry of Materials, 1997,9:2491-2498.
[16]
Pauly T R, Liu Y, Pinnvaia T J, et al. Textural mesoporosity and the catalytic activity of mesoporous molecular sieves with wormhole framework structures[J]. Journal of the American Chemical Society. 1999,121:8835-8842.
[17]
Lu C, Bai H, Su F, et al. Adsorption of carbon dioxide from gas streams via mesoporous spherical-silica particles[J]. Journal of the Air & Waste Management Association. 2010,60:489-496.
[18]
Wang X R, Li H Q, Liu H T, et al. AS-synthesized mesoporous silica MSU-1modified with tetraethylenepentamine for CO2 adsorption[J]. Microporous and Mesoporous Materials, 2011, 142:564-569.
Ma J J, Liu Q M, Chen D D. Carbon dioxide adsorption using amine-functionalized mesocellular siliceous foams[J]. Journal of Materials Science, 2014,49:7585-7596.
