Hydrothermal Synthesis of Ordered Mesoporous Silicas with Extraordinarily Ultra-low Dielectric Constants

doi:10.3969/j.issn.0251-0790.2012.09.006

Abstract

Abstract:

Ordered mesoporous silica samples with extraordinarily ultra-low dielectric constants(k) were hydrothermally synthesized at different temperatures(150—200℃) via soft-templates including amphiphilic triblock polymers of P123(PEO₂₀-PPO₇₀-PEO₂₀) and F127(PEO₁₀₆-PPO₇₀-PEO₁₀₆). The characterizations of XRD and N₂ adsorption-desorption isotherms show that these samples have ordered mesostructure, high BET surface area, large pore volume and uniform pore size.²⁹Si MAS NMR spectra show that the samples have much higher silica condensation degree than the ones synthesized at relatively low temperatures. More importantly, these samples exhibit extraordinarily ultra-low dielectric constant(k). For example, ordered mesoporous silica of SBA-15 synthesized at 200℃ gives k value as low as 1.31, which is interpreted by a collaborative effect of large pore volume with high silica condensation degree. These samples with extraordinarily ultra-low dielectric constants would be potentially important for applications of superior insulators in electronic industry.

Key words: Ordered mesoporous material, High temperature synthesis, Silica, Dielectric constant, Condensation degree

CLC Number:

O613

TrendMD:

LIU Fu-Jian, HAN Bing, CAO Yang, ZOU Yong-Cun, MENG Xiang-Ju, XIAO Feng-Shou. Hydrothermal Synthesis of Ordered Mesoporous Silicas with Extraordinarily Ultra-low Dielectric Constants[J]. Chem. J. Chinese Universities, 2012, 33(09): 1908.

References

[1] Peercy P. S.. Nature[J], 2000, 406(6799): 1023-1026

[2] Liu Y., Lew C. M., Sun M. W., Cai R., Wang J. L., Kloster G., Boyanov B., Yan Y. S.. Angew. Chem. Int. Ed.[J], 2009, 48(26): 4777-4780

[3] Volksen W., Miller R. D., Dubois G.. Chem. Rev.[J], 2010, 110(1): 56-110

[4] Seraji S., Wu Y., Forbess M., Limmer S. J., Chou T., Cao G. Z.. Adv. Mater.[J], 2000, 12(22): 1695-1698

[5] Lee W. W., Ho P. S.. MRS Bull.[J], 1997, 22(10): 19-52

[6] Eds: Lagendijk A., Treichel H., Uram K. J., Jones A. C.. Low-Dielectric Constant Materials Ⅱ[M], Pittsburgh: Materials Research Society, PA, 1997, Vol. 443

[7] International Technology Roadmap for Semiconductors. http: //www. itrs.net(accessed March 2008)

[8] Maex K., Baklanov M. R., Shamiryan D., Iacopi F., Brongersma S. H., Yanovitskaya Z. S.. J. Appl. Phys.[J], 2003, 93(11): 8793-8841

[9] International Technology Roadmap for Semiconductors, http://www.itrs.net(accessed May 2007)

[10] Ho P. S., Lee W. W., Leu J. J.. Low Dielectric Constant Materials for IC Applications[M], New York: Springer, 2003, Vol. 9

[11] Morgen M., Ryan E. T., Zhao J. H., Hu. C., Cho T. H., Ho P. S.. Annu. Rev. Mater. Sci.[J], 2000, 30: 645-680

[12] Jin C., Lin S., Wetzel J. T.. J. Electron. Mater.[J], 2001, 30(4): 284-289

[13] Dubois G., Volksen W., Miller R. D.; Eds.: Baklanov M., Maex K., Green M.. Dielectric Materials Research for Advanced Microelectronic Devices[M], New York: Wiley, 2007: 35-36

[14] Grill A.; Eds.: Baklanov M., Maex K., Green M.. Advanced Interconnects for ULSI Technology[M], New York: Wiley, 2007: 9-10

[15] Baskaran S., Liu J., Domansky K., Kohler N., Li X., Coyle C., Freyxell G. E., Thevutharampillai S., Williford R. E.. Adv. Mater.[J], 2000, 12(4): 291-294

[16] Zhao D., Yang P., Melosh N., Feng J. L., Chmelka B. F., Stucky G. D.. Adv. Mater.[J], 1998, 10(16): 1380-1385

[17] Nguyen C. V., Carter K. R., Hawker C. J., Hedrick J. L., Jaffe R. L., Miller R. D., Remenar J. F., Rhee H. W., Rice P. M., Toney M. F., Trollsas M., Yoon D. Y.. Chem. Mater.[J], 1999, 11(11): 3080-3085

[18] Shen L., Zeng K. Y., Wang Y. H., Narayanan B., Kumar R.. Microelectron. Eng.[J], 2003, 70(1): 115-124

[19] Puyrenier W., Rouessac V., Broussous L., Rébiscoul D., Ayral A.. Micropor. Mesopor. Mater.[J], 2007, 106(1-3): 40-48

[20] Mowat I. A., Lin X. F., Fister T., Kendall M., Chao G., Yang M. H.. Appl. Surf. Sci. [J], 2006, 252(19): 7182-7185

[21] Yang C. M., Cho A. T., Pan F. M., Tsai T. G., Chao K. J.. Adv. Mater.[J], 2001, 13(14): 1099-1102

[22] Tsai T. G., Cho A. T., Yang C. M., Pan F. M., Chao K. J.. J. Electrochem. Soc.[J], 2002, 149: F116-F121

[23] Hendricks N. H.. Mater. Res. Soc. Proc.[J], 1997, 443(11): 3-16

[24] Case C. B., Case C. J., Kornblit A., Mills M. E., Castillo D., Liu R.. Mater. Res. Soc. Proc.[J], 1997, 443(11): 177-185

[25] Maier G.. Prog. Polym. Sci.[J], 2001, 26(1): 3-65

[26] Veres J., Ogier S. D., Leeming S. W., Cupertino D. C., Khaffaf S. M.. Adv. Mater.[J], 2003, 15(3): 199-204

[27] Zhao G. F., Ishizaka T., Kasai H., Hasegawa M., Furukawa T., Nakanishi H., Oikawa H.. Chem. Mater.[J], 2009, 21(2): 419-424

[28] Hasegawa M., Horie K.. Prog. Polym. Sci.[J], 2001, 26(2): 259-335

[29] Wang Z. B., Wang H. T., Mitra A., Huang L. M., Yan Y. S.. Adv. Mater.[J], 2001, 13(10): 746-749

[30] XU Hong-Yao(徐洪耀), YAN Zheng-Quan(严正权), ZHANG Chao(张超), SU Xin-Yan(苏新艳), GUANG Shan-Yi(光善仪). Chem. J. Chinese Universities(高等学校化学学报)[J], 2011, 32(9): 1962-1969

[31] Wang Z. B., Mitra A., Wang H. T., Huang L. M., Yan Y. S.. Adv. Mater.[J], 2001, 13(18): 1463-1468

[32] Liu Y., Sun M. W., Lew C. M., Wang J. L., Yan Y. S.. Adv. Funct. Mater.[J], 2008, 18(12): 1732-1738

[33] Lew C. M., Li Z. J., Li S., Hwang S. J., Liu Y., Medina D. I., Sun M. W., Wang J. L., Davis M. E., Yan Y. S.. Adv. Funct. Mater.[J], 2008, 18(21): 3454-3460

[34] Li Z. J., Li S., Luo H. M., Yan Y. S.. Adv. Funct. Mater.[J], 2004, 14(20): 1019-1024

[35] Hunt H. K., Lew C. M., Sun M. W., Yan Y. S., Davis M. E.. Micropor. Mesopor. Mater.[J], 2010, 130(1-3): 49-55

[36] Lew C. M., Liu Y., Day B., Kloster G. M., Tiznado H., Sun M. W., Zaera F., Wang J. L., Yan Y. S.. Langmuir[J], 2009, 25(9): 5039-5044

[37] Zhu Y. Z., Müller T. E., Lercher J. A.. Adv. Funct. Mater.[J], 2008, 18(21): 3427-3433

[38] Han Y., Li D. F., Zhao L., Song J. W., Yang X. Y., Li N., Di Y., Li J. C., Wu S., Xu X. Z., Meng X. J., Lin K. F., Xiao F. S.. Angew. Chem. Int. Ed.[J], 2003, 42(31): 3633-3637

[39] Li D. F., Han Y., Song J., Zhao L., Xu X. Z., Di Y., Xiao F. S.. Chem. Eur. J.[J], 2004, 10(23): 5911-5922

[40] Xiao N., Wang L., Liu S., Zou Y. C., Wang C. Y., Ji. Y. Y., Song J. W., Li F., Meng X. J., Xiao F. S.. J. Mater. Chem.[J], 2009, 19(5): 661-665

[41] Zhang P. L., Wu Z. F., Xiao N., Ren L. M., Meng X. J., Wang C. Y., Li F., Li Z. Q., Xiao F. S.. Langmuir[J], 2009, 25(22): 13169-13175

[42] Liu F. J., Li C. J., Ren L. M., Meng X. J., Zhang H., Xiao F. S.. J. Mater. Chem.[J], 2009, 19(42): 7921-7928

[43] Zhao D. Y., Feng J. L., Huo Q. S., Melosh N., Fredrickson G. H., Chmelka B. F., Stucky G. D.. Science[J], 1998, 279(5350): 548-552

[44] Zhao D. Y., Huo Q. S., Feng J. L., Chmelka B. F., Stucky G. D.. J. Am. Chem. Soc.[J], 1998, 120(24): 6024-6036

[45] Zhu J., You W. S., Zhu Z. M., Sun Z. G., Zhang L. C., Gu Y. P.. Chem. Res. Chinese Universities[J], 2005, 21(3): 264-267