用于燃烧前CO2捕集的微孔Nb2O5膜的制备及其水热稳定性能

doi:10.3969/j.issn.0438-1157.2013.11.024

化工学报 ›› 2013, Vol. 64 ›› Issue (11): 4060-4067.DOI: 10.3969/j.issn.0438-1157.2013.11.024

用于燃烧前CO₂捕集的微孔Nb₂O₅膜的制备及其水热稳定性能

陈加伟, 陈慧如, 漆虹, 徐南平

南京工业大学膜科学技术研究所, 材料化学工程国家重点实验室, 江苏南京 210009

收稿日期:2013-03-19 修回日期:2013-06-01 出版日期:2013-11-05 发布日期:2013-11-05
通讯作者: 漆虹
作者简介:陈加伟(1989-),男,硕士研究生。
基金资助:
国家自然科学基金项目(20906047,21276123);国家高技术研究发展计划项目(2012AA03A606);江苏省高校自然科学研究计划项目(11KJB530006);江苏省“六大人才高峰”项目;材料化学工程国家重点实验室自主课题(ZK201002)。

Fabrication and hydrothermal stability of microporous Nb₂O₅ membrane for pre-combustion capture of CO₂

CHEN Jiawei, CHEN Huiru, QI Hong, XU Nanping

State Key Laboratory of Materials-Oriented Chemical Engineering, Membrane Science and Technology Research Center, Nanjing University of Technology, Nanjing 210009, Jiangsu, China

Received:2013-03-19 Revised:2013-06-01 Online:2013-11-05 Published:2013-11-05
Supported by:
supported by the National Natural Science Foundation of China(20906047,21276123),the High-tech Research and Development Program of China(2012AA03A606),the Natural Science Research Plan of Jiangsu Universities(11KJB530006),the “Summit of the Six Top Talents” Program of Jiangsu Province and the State Key Laboratory of Materials-Oriented Chemical Engineering(ZK201002).

摘要/Abstract

摘要： 以五正丁氧基铌为前驱体,通过溶胶-凝胶法制备出稳定的Nb₂O₅聚合溶胶,详细考察了溶胶制备过程参数(体系酸度、水解比、反应温度、反应时间和螯合剂用量)对溶胶尺寸、稳定性以及制备重复性的影响。采用平均粒径为4.8 nm的Nb₂O₅溶胶,通过浸浆法在平均孔径为3 nm的γ-Al₂O₃中孔膜上制备出Nb₂O₅微孔膜。利用TG、XRD、NH₃吸附-脱附、CO₂吸附、吡啶吸附傅里叶变换红外光谱(Py-IR)和单组分气体渗透实验等手段对Nb₂O₅粉体及微孔膜的性能进行了表征,结果表明:在200℃、0.3 MPa条件下,350℃烧成的微孔Nb₂O₅膜对H₂的渗透率和H₂/CO₂的理想分离因子分别为3.1×10^-9 mol·m^-2·s^-1·Pa^-1和21。此外,微孔Nb₂O₅膜经150 kPa的水蒸气处理8 h后,膜的渗透性能以及H₂/CO₂理想选择性基本保持不变。

关键词: 微孔陶瓷膜, Nb₂O₅, CO₂捕集, 水热稳定性

Abstract: Polymeric Nb₂O₅ sols were successfully synthesized via sol-gel process by using niobium penta(n)butoxide as a precursor.Effects of synthesis parameters,including pH of system,hydrolysis ratio,reaction temperature,reaction time and chelating agent,on the state and size of Nb₂O₅ sols were investigated in detail.Microporous Nb₂O₅ membranes were deposited on defect-free γ-alumina membranes with an average pore size of ca.3 nm,by using polymeric Nb₂O₅ sol with an average size of 4.8 nm.The properties of Nb₂O₅ powder and the supported Nb₂O₅ membranes were characterized by TG,XRD,NH₃ adsorption-desorption,CO₂ adsorption,Fourier-transform infrared spectroscopy of pyridine adsorption(Py-IR)and single gas permeance test.Results showed that the single hydrogen permeance and H₂/CO₂ permselectivity of 350℃-calcined microporous Nb₂O₅ membrane were 3.1×10^-9 mol·m^-2·s^-1·Pa^-1 and 21,respectively,measured at 200℃ and 0.3 MPa.The single gas permeance and H₂/CO₂ permselectivity of the membrane remained fairly stable after in-situ exposure to 150 kPa steam for 8 h.

Key words: microporous ceramic membrane, Nb₂O₅, CO₂ capture, hydrothermal stability

中图分类号:

TQ028

陈加伟, 陈慧如, 漆虹, 徐南平. 用于燃烧前CO₂捕集的微孔Nb₂O₅膜的制备及其水热稳定性能[J]. 化工学报, 2013, 64(11): 4060-4067.

CHEN Jiawei, CHEN Huiru, QI Hong, XU Nanping. Fabrication and hydrothermal stability of microporous Nb₂O₅ membrane for pre-combustion capture of CO₂[J]. CIESC Journal, 2013, 64(11): 4060-4067.

参考文献 24

[1]	Bredesen R,Peters T A.Membranes in energy systems with CO2 capture[J].Membranes for Energy Conversion,2008,2:217-244
[2]	Mangalapally H P,Notz R,Hoch S,Asprion N,Sieder G,Garcia H,Hasse H.Pilot plant experimental studies of post combustion CO2 capture by reactive absorption with MEA and new solvents[J].Energy Procedia,2009,1(1):963-970
[3]	Ho M T,Allinson G W,Wiley D E.Reducing the cost of CO2 capture from flue gases using pressure swing adsorption[J].Ind.Eng.Chem.Res.,2008,47:4883-4890
[4]	Ho M T,Allinson G W,Wiley D E.Reducing the cost of CO2 capture from flue gases using membrane technology[J].Ind.Eng.Chem.Res.,2008,47:1562-1568
[5]	Bernardo P,Drioli E,Golemme G.Membrane gas separation:a review/state of the art[J].Ind. Eng. Chem.Res.,2009,48(10):4638-4663
[6]	Mallada R,Menéndez M.Inorganic Membranes Synthesis,Characterization and Applications[M].Amsterdam:Elsevier,2008:217-245
[7]	de Vos R M,Verweij H.High-selectivity,high-flux silica membranes for gas separation[J].Science,1998,279(5357):1710-1711
[8]	Boffa V,Blank D H A,ten Elshof J E.Hydrothermal stability of microporous silica and niobia-silica membranes[J].J.Membr.Sci.,2008,319(1/2):256-263
[9]	Qi Hong,Han Jing,Xu Nanping,Bouwmeester H J M. Hybrid organic-inorganic microporous membranes with high hydrothermal stability for the separation of carbon dioxide[J].ChemSusChem,2010,3(12):1375-1378
[10]	Uhlmann D,Liu Shaomin,Ladewig B P,Diniz da Costa J C.Cobalt-doped silica membranes for gas separation[J].J.Membr.Sci.,2009,326(2):316-321
[11]	Kanezashi M,Asaeda M.Hydrogen permeation characteristics and stability of Ni-doped silica membranes in steam at high temperature[J].J.Membr.Sci.,2006,271(1/2):86-93
[12]	Coterillo C C,Yokoo T,Yoshioka T,Tsuru T,Asaeda M.Synthesis and characterization of microporous ZrO2 membranes for gas permeation at 200℃[J].Sep. Sci. Technol.,2011,46(8):1224-1230
[13]	Kreiter R,Rietkerk M D A,Bonekamp B C,van Veen H M,Kessler V G,Vente J F.Sol-gel routes for microporous zirconia and titania membranes[J].J.Sol-Gel Sci. Technol.,2008,48(1/2):203-211
[14]	Nowak I,Ziolek M.Niobium compounds:preparation,characterization,and application in heterogeneous catalysis[J].Chem.Rev.,1999,99:3603-3624
[15]	Ziolek M.Niobium-containing catalysts-the state of the art[J].Catal.Today,2003,78:47-64
[16]	Okuhara T.Water-tolerant solid acid catalysts[J].Chem. Rev.,2002,102:3641-3666
[17]	Qi Hong(漆虹),Han Jing(韩静),Jiang Xiaoluo(江晓骆),Tao Zhen(陶振),Xing Weihong(邢卫红),Fan Yiqun(范益群).Hydrothermal stability of microporous SiO2 membranes[J].The Chinese Journal of Process Engineering(过程工程学报),2010,10(1):161-166
[18]	Braga V S,Dias J A,Dias S C L,de Macedo J L.Catalyst materials based on Nb2O5 supported on SiO2-Al2O3 preparation and structural characterization[J].Chem. Mater.,2005,17:690-695
[19]	Kanezashi M,Kawano M,Yoshioka T,Tsuru T.Organic-inorganic hybrid silica membranes with controlled silica network size for propylene/propane separation[J].Ind. Eng. Chem.Res.,2012,51(2):944-953
[20]	Castricum H L,Sah A,Kreiter R,Blank D H A,Vente J F,ten Elshof J E.Hydrothermally stable molecular separation membranes from organically linked silica[J].J.Mater.Chem.,2008,18(18):2150-2158
[21]	Castricum H L,Kreiter R,van Veen H M,Blank D H A,Vente J F,ten Elshof J E.High-performance hybrid pervaporation membranes with superior hydrothermal and acid stability[J].J.Membr.Sci.,2008,324(1/2):111-118
[22]	Qi Hong,Han Jing,Xu Nanping.Effect of calcination temperature on carbon dioxide separation properties of a novel microporous hybrid silica membrane[J].J. Membr.Sci.,2011,382(1/2):231-237
[23]	Boffa V,ten Elshof J E,Petukhov A V,Blank D H A.Microporous niobia-silica membrane with very low CO2 permeability[J].ChemSusChem,2008,1(5):437-443
[24]	He Jie(何杰),Fan Yining(范以宁).Dispersion and acidity of niobia on Nb2O5/γ-Al2O3[J].Acta.Phys.-Chim.Sin.(物理化学学报),2010,26(3):679-684

用于燃烧前CO₂捕集的微孔Nb₂O₅膜的制备及其水热稳定性能

Fabrication and hydrothermal stability of microporous Nb₂O₅ membrane for pre-combustion capture of CO₂

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