不同有机胺修饰MCM-41的CO<sub>2</sub>吸附性能和热稳定性

刘之琳; 滕阳; 张锴; 曹晏; 潘伟平

不同有机胺修饰MCM-41的CO₂吸附性能和热稳定性

刘之琳¹,
滕阳¹,
张锴^1,,
曹晏^1,2,
潘伟平^1,2

1.
华北电力大学能源化工研究中心, 北京 102206;
2.
美国西肯塔基大学燃烧科学与环境技术研究所美国 42101

基金项目: 国家自然科学基金 (51061130538); 国家高技术发展研究计划(863计划, 2012AA06A115); 111引智计划(B12034).

详细信息

通讯作者:
张锴, E-mail: kzhang@ncepu.edu.cn.

中图分类号: O647.33
计量
- 文章访问数: 2322
- HTML全文浏览量: 23
- PDF下载量: 638
- 被引次数: 0
出版历程
- 收稿日期: 2012-09-29
- 修回日期: 2012-12-11
- 刊出日期: 2013-04-30

CO₂ adsorption properties and thermal stability of different amine-impregnated MCM-41 materials

1.
Center of Chemical Engineering and Technology for Energy, North China Electric Power University, Beijing 102206, China;
2.
The Institute of Combustion Science and Environmental Technology, Western Kentucky University 42101, USA

摘要

摘要: 将乙二胺(EDA,60 g/mol)、四乙烯五胺(TEPA,189 g/mol)和两种聚乙烯亚胺600(PEI600g/mol; PEI1800g/mol)分别负载在MCM-41上制备氨基功能化介孔材料,研究其对CO₂的吸附性能和热稳定性.结果表明,除了EDA-MCM41,其他三种材料随着胺分子量增大CO₂吸附性能下降,但是热稳定性却有所提高,其中,TEPA-MCM41的吸附容量最大,达到2.7 mmol/g.同时发现,乙二胺在制备过程中随溶剂挥发而难以完全负载在MCM-41上.在纯N₂气氛和再生温度100 ℃条件下,经10次循环实验后,TEPA-MCM41的吸附能力下降了7.4%,而PEI600-MCM41和PEI1800-MCM41吸附能力保持不变,且质量变化在1%以内,表现出良好的再生稳定性.采用80%CO₂/20%N₂对吸附饱和的材料进行再生,四种材料的再生温度将提高到160 ℃以上,高分子量PEI600-MCM41和PEI1800-MCM41相比于TEPA-MCM41具有更好的热稳定性.
- 氨基功能化 /
- CO₂吸附 /
- 热稳定性
Abstract: The adsorption properties of CO₂ on MCM-41 mesoporous materials impregnated with ethylenediamine (EDA), tetraethylenepentamine (TEPA) and two kinds of polyethylenimines (PEI600 and PEI1800), respectively, were studied with mass spectrometry (MS) and thermogravimetry (TG) techniques. The sample obtained by impregnating EDA (EDA-MCM-41) showed a low CO₂ adsorption capacity due to the ready volatilization of EDA, while those samples prepared by TEPA (TEPA-MCM-41), PEI600 (PEI600-MCM-41) or PEI1800 (PEI1800-MCM-41) exbibit higher adsorption capacity and thermal stability although the adsorption capacity decreased with increasing molecular weight of amines. A maximum CO₂ adsorption capacity of 2.7 mmol/g was achieved on the TEPA-MCM-41 with 40% TEPA. When this sample was regenerated at 100 ℃ under pure nitrogen atmosphere, its CO₂ adsorption capacity was decreased by 7.4% after ten recycles in contrast to less than 1% for both PEI600-MCM-41 and PEI1800-MCM-41. However, when the regeneration atmosphere was changed to 80% CO₂/20% N₂, the regeneration temperature should be be increased to more than 160 ℃ for all the samples despite that PEI-MCM-41 showed high thermal stability than TEPA-MCM-41.
- amine-based MCM-41 /
- CO₂ adsorption /
- thermal stability

HTML全文

参考文献(35)

SONG C.Global challenges and strategies for control, conversion and utilization of CO₂ for sustainable development involving energy, catalysis, adsorption and chemical processing[J] . Catal Today, 2006, 115(1): 2-32.

ZHAO X S, LU G Q, WHITTAKER A K, MILLAR G J, ZHU H Y. Comprehensive study of surface chemistry of MCM-41 using 29Si CP/MAS NMR, FTIR, pyridine-TPD, and TGA[J]. J Chem Phys, 1997, 101(33): 6525-6531.

HUANG H Y, YANG R T, CHINN D, MUNSON C L. Amine-grafted MCM-48 and silica xerogel as superior sorbents for acidic gas removal from natural gas[J]. Ind Eng Chem Res, 2003, 42(12): 2427- 2433.

HARLICK P J E, SAYARI A. Applications of pore-expanded mesoporous silicas. 3-triamine silane grafting for enhanced CO₂ adsorption[J]. Ind Eng Chem Res, 2006, 45(9): 3248-3255.

WEI J W, SHI J J, PAN H, SU Q F, ZHU J B, SHI Y. Hermal and hydrothermal stability of amino-functionalized SBA-16 and promotion of hydrophobicity by silylation[J] . Micro Mesoporous Mater, 2009, 117(3):596-602.

HICKS J C, DRESE J H, FAUTH D J, GRAY M L, Qi G G, JONES C W. Designing adsorbents for CO₂ capture from flue gas-hyperbranched aminosilicas capable of capturing CO₂ reversibly[J]. J Am Chem Soc, 2008, 130(10): 2902-2903.

KNOFEL C, DESCARPENTRIES J, BENZAOUIA A, ZELENAK V, MORNET S, LLEWELLYN P L, HORNEBECQ V. Functionalised micro-/mesoporous silica for the adsorption of carbon dioxide[J]. Microporous Mesoporous Mater, 2007, 99(1): 79-85.

LIU X W, ZHOU L, FU X, SUN Y, SU W, ZHOU Y P. Adsorption and regeneration study of the mesoporous adsorbent SBA-15 adapted to the capture/separation of CO₂ and CH₄[J]. Chem Eng Sci, 2007, 62(4) : 1101-1110.

CHANG A C C, CHUANG S S C, GRAY M, SOONG Y. In-situ infrared study of CO₂ adsorption on SBA-15 grafted with γ-(aminopropyl) triethoxysilane[J]. Energy Fuels, 2003, 17(2): 468-473.

XU X H, WU H S, DUAN J F, WANG F, JIN F, LEE Z Y. Statistical approach for the optimal deposition of Cr underlayer for SmCo/Cr magnetic films[J]. Appl Sur Sci, 2003, 218(1): 29-33.

KNOWLES G P, GRAHAM J V, DELANEY S W, CHAFFEE A L. Aminopropyl-functionalized mesoporous silicas as CO₂ adsorbents[J]. Fuel Process Technol, 2005, 86(14/15): 1435-1448.

HUANG H Y, YANG R, CHINN D. Amine grafted MCM-48 and silica xerogel as superior sorbents for acidic gas removal from natural gas[J]. Ind Eng Chem Res, 2003, 42(12): 2427-2433.

KHATRI RAJESH A, CHUANG STEVEN S C,SOONG Y. Thermal and Chemical Stability of Regenerable Solid Amine Sorbent for CO₂ Capture[J]. Energy Fuels, 2006, 20(4): 1514-1520.

WEI J W, LIAO L, XIAO Y, ZHANG P, SHI Y. Capture of carbon dioxide by amine-impregnated as-synthesized MCM-41[J]. J Environ Sci.2010, 22(10) : 1558-1563.

XU X, SONG C, ANDRESEN J M, MILLER B G,SCARONI A W.Novel polyethylenimine-modified mesoporous molecular sieve of MCM-41 type as high-capacity adsorbent for CO₂ capture [J] .Energy Fuels , 2002, 16(6): 1463-1469.

XU X C, SONG C S, ANDRESEN JOHN M , MILLER BRUCE G, SCARONI A W. Preparation and characterization of novel CO₂ "molecular basket" adsorbents based on polymer-modified mesoporous molecular sieve MCM-41[J]. Microporous Mesoporous Mater, 2003, 62(1): 29-46.

YUE M B, CHUN Y, CAO Y,DONG X, ZHU J H. Novel CO₂-capturer derived from the as-prepared SBA-15 occluded by template[J]. Adv Func Mater, 2006, 16(13): 1717-1722.

HEYDARI-GORGI A, BELMABKHOUT Y, SAYARI A. Polyethylenimine-impregnated mesoporous silica: Effect of amine loading and surface alkyl chains on CO₂ adsorption[J]. Langmuir, 2011, 27(20): 12411-12416.

GRAY M L, CHAMPAGNE K J, FAUTH D. Performance of immobilized tertiary amine solid sorbents for the capture of carbon dioxide[J]. Int J Greenhouse Gas Control, 2008, 2(1): 3-8.

SON W, CHOI J, AHN W. Adsorptive removal of carbon dioxide using polyethyleneimine-loaded mesoporous silica materials[J]. Microporous Mesoporous Mater. 2008, 113(1-3): 31-40.

闻霞, 孙楠楠, 李碧, 李军平, 王峰, 赵宁, 肖福魁, 魏伟, 孙予罕, 任泽厚, 郭金刚, 王志杰, 李庆, 吴志斌. MgO /Al₂O₃吸附剂对CO₂动态吸附性能的研究[J]. 燃料化学学报, 2010, 38(2): 247-251. (WEN Xia, SUN Nan-nan, LI B, LI Jun-ping, WANG Feng, ZHAO Ning, XIAO Fu-ku,WEI Wei,SUN Yun-han, REN Ze-hou, GUO Jin-gang, WANG Zhi-jie, LI Qing, WU Zhi-bin. Dynamic adsorption study of CO₂ adsorption by MgO /Al₂O₃[J]. Journal of Fuel Chemistry and Technology, 2010, 38(2): 247-251. )

李碧, 闻霞, 赵宁, 王秀枝, 魏伟, 孙予罕, 任泽厚, 王志杰. 高稳定性介孔MgO-ZrO₂ 固体碱的制备及其高温CO₂ 吸附性能[J]. 燃料化学学报, 2010, 38( 4 ): 473-477. (LI Bi, WEN Xia, ZHAO Ning, WANG Xiu-zhi, WEI Wei, SUN Yu-han, REN Ze-hou, WANG Zhi-jie. Preparation of high stability MgO-ZrO₂ solid base and its high temperature CO₂ capture properties[J]. Journal of Fuel Chemistry and Technology, 2010, 38(4): 473-477.

徐如人, 庞文琴. 分子筛与多孔材料化学[M]. 北京: 科学出版社, 2004. (XU Ru-ren, PANG Xiu-qing. Chemistry: Zeolites and Porous[M]. Beijing: Science Press, 2004)

付新, 王冬华. 聚乙烯亚胺修饰的介孔材料对CO₂的吸附性能[J]. 化工新型材料, 2011, 39(11): 90-92. (FU Xin, WANG Dong-hua.CO₂ adsorption on mesoporous molecular sieves modified by polyethylenemine[J]. New Chemical Materials, 2011, 39(11): 90-92).

HIYOSHI N, YOGO K, YASHIMA T. Adsorption characteristics of carbon dioxide on organically functionalized SBA-15[J]. Microporous Mesoporous Mater, 2005, 84(1/3): 357-365.

KNOWLES G P, GRAHAM J V, DELANEY S W, CHAEE A L. Aminopropyl-functionalized mesoporous silicas as CO₂ adsorbents. Fuel Process Technol[J], 2005, 86(14/15): 1435-1448.

YAN X L, ZHANG L, ZHANG Y, QIAO K, YAN Z F, KOMARNENI S. Amine-modified mesocellular silica foams for CO₂capture[J]. Chem Eng J, 2011, 168(2): 918-924.

赵会玲,胡军,汪建军,周丽绘,刘洪. 介孔材料氨基表面修饰及其对CO₂ 的吸附性能[J]. 物理化学学报, 2007, 23(6): 801- 806. (ZHAO Hui-Ling, HU Jun, WANG Jian-Jun, ZHOU Li-Hui, LIU Hong-Lai. CO₂ capture by the amine-modified mesoporous materials[J]. Acta Physico-chimica Sinica , 2007, 23(06): 801-806.)

WANG X R, LI H Q, LIU H T, HOU X J. AS-synthesized mesoporous silica MSU-1 modified with tetraethylenepentamine for CO₂ adsorption[J]. Microporous Mesoporous Mater.2011, 142: 564-569.

LIU L C, LI H Q, ZHANG Y. A comparative study on catalytic performances of chromium incorporated and supported mesoporous MSU-x catalysts for the oxidehydrogenation of ethane to ethylene with carbon dioxide[J]. Catal Today, 2006, 115(1/4): 235-241.

康平平, 宋文生, 韩冰冰, 许双双. 乙二胺基乙磺酸钠的合成与表征[J]. 有机化学, 2009. 29(6): 904-908 (KANG Ping-ping, SONG Wen-sheng, HAN Bing-bing. XU Shuang-shuang. Synthesis and characterization of aliphatic diamine sulphonate[J]. Chinese Journal of Organic Chemistry, 2009, 29(6): 904-908.)

YUE M B, SUN L B, CAO Y, WANG Y, WANG Z J, ZHU J H. Efficient CO₂ capturer derived from as-synthesized MCM-41 modified with amine[J].Chem Euro J, 2008, 14(11): 3442-3451

KHATRI R, CHUANG S C, SOONG Y, GRAY M. Carbon dioxide capture by diamine-grafted SBA-15: A combined fourier transform infrared and mass spectrometry study [J]. Ind Eng Chem Res, 2005, 44(10): 3702-3708.

WANG X X, SCHWARTZ V, CLARK J C, MA M L, OVERBURY S H, XU X C, SONG C S. Infrared study of CO₂ sorption over "Molecular Basket" sorbent consisting of polyethylenimine-modified mesoporous molecular sieve[J].J Phy Chem, 2009, 113(17): 7260-7268.

GOEPPERT A, CZAUN M, MAY R B, PRAKASH G K S, OLAH G A, NARAYANAN S R. Carbon dioxide capture from the air using a polyamine based regenerable solid adsorbent[J]. J Am Chem Soc, 2011, 133(50): 20164-20167.

施引文献

资源附件(0)

访问统计