快速制备高掺杂CuO/SiO2复合气凝胶

doi:10.3866/PKU.WHXB201209282

Abstract

Abstract:

Highly doped CuO/SiO₂ composite aerogels were prepared via a propylene oxide pre-reaction method with acetonitrile as solvent. In a typical synthesis process, tetramethoxysilane (TMOS), acetonitrile, deionized water, and propylene oxide were mixed together for pre-reaction. The solutions were then mixed with a CuCl2 acetonitrile-water solution, with added propylene oxide. The mixed solutions were transformed to the wet gels after being kept in the oven for 0.5 h at 35℃. The dark monolithic CuO/SiO₂ composite aerogels were obtained after drying with supercritical CO₂ and following thermal treatment. The density, specific surface area, average doping concentration, and compression modulus of the final aerogel samples were about 180 mg·cm^-3, 625 m²·g^-1, 19.91%± 2.42% (Cu:Si molar ratio), and 1.639 MPa, respectively. The aerogels, which were ideal materials for backlight targets, featured good formability and uniform dispersion. The gelation mechanism was also discussed by comparing our typical synthetic process with reference experiments. The results demonstrated that the reaction rates of the two precursors were balanced by changing the solvent and using the propylene oxide pre-reaction method, which realized the co-gelation. In addition, the method may inspire new synthetic ideas for preparation of other metal-oxide/silica composite aerogels.

Key words: Pre-reaction, Highly doping, Copper oxide, Composite aerogel, Propylene oxide, Co-gelation

MSC2000:

O648

XU Wei-Wei, DU Ai, TANG Jun, CHEN Ke, ZOU Li-Ping, ZHANG Zhi-Hua, SHEN Jun, ZHOU Bin. Rapid Preparation of Highly Doped CuO/SiO₂ Composite Aerogels[J].Acta Phys. -Chim. Sin., 2012, 28(12): 2958-2964.

References

(1) Chen, L.W.; Gan, L. H. Chemistry 1997, 8, 21. [陈龙武, 甘礼华. 化学通报, 1997, 8, 21.]
(2) Zu, G. Q.; Shen, J.;Wei, X. Q.; Ni, X. Y.; Zhang, Z. H.;Wang,J. C.; Liu, G.W. J. Non-Cryst. Solids 2011, 357, 2903. doi: 10.1016/j.jnoncrysol.2011.03.031
(3) Xu, Z. J.; Gan, L. H.; Pang, Y. C.; Chen, L.W. Acta Phys. -Chim. Sin. 2005, 21, 221. [徐子颉, 甘礼华, 庞颖聪,陈龙武. 物理化学学报, 2005, 21, 221.] doi: 10.3866/PKU.WHXB20050204
(4) Du, A.; Zhou, B.; Zhong, Y. H.; Zhu, X. R.; Gao, G. H.;Wu, G.M.; Zhang, Z. H.; Shen, J. J. Sol-Gel Sci. Technol. 2011, 58,225. doi: 10.1007/s10971-010-2381-8
(5) Zhao, Z. Q.; Jiao, X. L.; Chen, D. R. J. Mater. Chem. 2009, 19,3078. doi: 10.1039/b819849g
(6) Du, A.; Zhou, B.; Shen, J.; Gui, J. Y.; Liu, C. Z.; Fan, G. L.;Zhang, Z. H. Energy Sci. Technol. 2010, 44, 1006. [杜艾,周斌, 沈军, 归佳寅, 刘春泽, 范广乐, 张志华. 原子能科学技术, 2010, 44, 1006.]
(7) Du, A.; Zhou, B.; Shen, J.; Gui, J. Y.; Zhong, Y. H.; Liu, C. Z.;Zhang, Z. H.;Wu, G. M. New J. Chem. 2011, 35, 1096. doi: 10.1039/c0nj00909a
(8) Rotter, H.; Landau, M.V.; Carrera, M.; Goldfarb, D.; Herskowitz,M. Appl. Catal. B 2004, 47, 111. doi: 10.1016/j.apcatb.2003.08.006
(9) Wittwer, V. J. Non-Cryst. Solids 1992, 145, 233. doi: 10.1016/S0022-3093(05)80462-4
(10) Zhou, B.; Shen, J.;Wu, G. M.; Sun, Q.; Huang, Y. D.;Wang, J.Atmoic Energy Sci. Technol. 2004, 38, 125. [周斌, 沈军,吴广明, 孙骐, 黄耀东, 王钰. 原子能科学技术, 2004, 38,125.]
(11) Du, A.; Zhou, B.;Wu, Y. H.; Xiao, S. F.; Liu, C. Z.; Shen, J.; Ni,X. Y. Atomic Energy Sci. Technol. 2008, 42, 794. [杜艾,周斌, 吴越华, 肖淑芳, 刘春泽, 沈军, 倪星元. 原子能科学技术, 2008, 42, 794.]
(12) Chen, L.W.; Gan, L. H.; Hou, X. H. Acta Phys. -Chim. Sin.2003, 19, 819. [陈龙武, 甘礼华, 侯秀红. 物理化学学报,2003, 19, 819.] doi: 10.3866/PKU.WHXB20030908
(13) Gui, J. Y.; Zhou, B.; Zhong, Y. H.; Du, A.; Shen, J. J. Sol-Gel Sci. Technol. 2011, 58, 470. doi: 10.1007/s10971-011-2415-x
(14) Tillotson, T. M.; Hrubesh. L.W. J. Non-Cryst. Solids 1992, 145,44. doi: 10.1016/S0022-3093(05)80427-2
(15) Abecassis-Wolfovich, M.; Rotter, H.; Landau, V.; Korin, E.;Erenburg, A. L.; Mogilyansky, D.; Garshtein, E. Stud. Surf. Sci. Catal. 2003, 146, 247. doi: 10.1016/S0167-2991(03)80373-7
(16) Gash, A. E.; Tillotson, T. M.; Satcher, J. H., Jr.; Hrubesh, L.W.;Simpson, R. L. J. Non-Cryst. Solids 2001, 285, 22.
(17) Skapin, T.; Kemnitz, E. J. Non-Cryst. Solids 1998, 225, 163.doi: 10.1016/S0022-3093(98)00037-4
(18) Du, A.; Zhou, B.; Li, L. X.; Zhu, X. R.; Li, Y. N.; Shen, J.; Gao,G. H.; Zhang, Z. H.;Wu, G. M. Atomic Energy Sci. Technol.2012, 46, 842. [杜艾, 周斌, 李龙翔, 朱秀榕, 李宇农,沈军, 高国华, 张志华, 吴广明. 原子能科学技术, 2012, 46,842.]
(19) Mohanan, J. L.; Brock, S. L. Chem. Mater. 2003, 15, 2567. doi: 10.1021/cm021741x
(20) Oh, Y. J.; Nam, B. A. Solid State Sci. 2011, 13, 1579. doi: 10.1016/j.solidstatesciences.2011.06.002
(21) Zheng, M. F.; Zhao, T. B.; Xu,W. G.; Li, F. Y.; Yang, Y. J. Sol- Gel Sci. Technol. 2006, 39, 151. doi: 10.1007/s10971-006-9172-2
(22) Feng, Y. Y.; Gu, M.; Du, Y. G. Acta Chim. Sin. 2012, 70, 831.[冯砚艳, 辜敏, 杜云贵, 化学学报, 2012, 70, 831.]doi: 10.6023/A1111151
(23) Gan, L. H.; Li, G. M.; Yue, T. Y.; Zhang, M.;Wu, J.W.; Chen,L.W. Acta Phys. -Chim. Sin. 1999, 15, 588. [甘礼华, 李光明,岳天仪, 张明, 吴建文, 陈龙武. 物理化学学报, 1999, 15,588.] doi: 10.3866/PKU.WHXB19990703
(24) Clapsaddle, B. J.; Sprehn, D.W.; Gash, A. E.; Satcher, J. H., Jr.;Simpson, R. L. J. Non-Cryst. Solids 2004, 350, 173. doi: 10.1016/j.jnoncrysol.2004.06.025
(25) Li, G. P.; Li, N. K.; Luo, Y. J.; Gao, K.; Chen, R. J. J. Beijing Inst. Technol. 2011, 31, 1335. [李国平, 李念珂, 罗运军,高坤, 陈人杰. 北京理工大学学报, 2011, 31, 1335.]
(26) Gash, A. E.; Satcher, J. H., Jr.; Simpson, R. L. J. Non-Cryst. Solids 2004, 350, 145. doi: 10.1016/j.jnoncrysol.2004.06.030
(27) Rao, A. V.; Hegde, N. D.; Hirashima, H. J. Colloid Interface Sci.2007, 305, 124. doi: 10.1016/j.jcis.2006.09.025
(28) Sing, K. S.W.; Everett, D. H.; Haul, R. A.W. Pure Appl. Chem.1985, 57, 603. doi: 10.1351/pac198557040603

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Rapid Preparation of Highly Doped CuO/SiO₂ Composite Aerogels

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Rapid Preparation of Highly Doped CuO/SiO₂ Composite Aerogels