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研究生: 楊承慈
Cheng-Tzu Yang
論文名稱: 氮化鎵奈米柱結構於中孔洞沸石粉末的製備與光譜分析
Formation of Arrays of Gallium Nitride Nanorods within Mesoporous Silica SBA-15
指導教授: 黃暄益
Professor Michael H. Huang
口試委員:
學位類別: 碩士
Master
系所名稱: 理學院 - 化學系
Department of Chemistry
論文出版年: 2005
畢業學年度: 93
語文別: 英文
論文頁數: 73
中文關鍵詞: 中孔洞二氧化矽氮化鎵奈米柱
外文關鍵詞: Mesoporous Silica, gallium nitride, nanorod
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  • 本論文旨在研究,利用中孔洞分子篩SBA-15之孔道控制Ⅲ-Ⅴ族氮化鎵奈米柱的生成,及探討氮化鎵奈米柱之光學性質。由於SBA-15具有均勻的孔道大小,故可用於當作模板以控制半導體材料的生成大小及形狀。本篇論文利用濕式含浸法將溶於甲苯的三氯化鎵溶液填充入孔道表面已修飾過甲基之SBA-15的孔道內,再將其於高溫下燒結以生成氮化鎵奈米柱,所生成之氮化鎵奈米柱之直徑介於6至7.5奈米而長度可達數百奈米。其後,以氟化氫水溶液移除氮化鎵奈米柱外所包覆的SBA-15,再將其分散於水溶液中以研究其光學特性。光致激發螢光光譜的結果顯示其具有一根近能隙峰位於375奈米與兩根施子-受子複合對與一次和三次縱向光聲子偶合鋒分別位於395奈米與415奈米,且我們可於335至360奈米間得到一根受量子局限效應引響而生成的藍位移放射光。


    We report the first formation of arrays of GaN nanorods inside the nanoscale channels of mesoporous silica SBA-15. GaCl3 dissolved in toluene was incorporated into the methyl group-functionalized SBA-15 powder. The pore surfaces functionalized with methyl groups should facilitate the impregnation with GaCl3. Formation of GaN nanorod arrays within SBA-15 was carried out by heating the powder to 700 °C for 3 h under nitrogen atmosphere, followed by ammonolysis at 900 °C for 5 h. □-Ga2O3, an unusual phase for Ga2O3, formed after the first thermal process and was converted into wurtzite GaN during ammonolysis. The final products have been characterized by FT-IR spectra, powder XRD patterns, TEM images and SAED patterns, EDS analysis, and nitrogen adsorption–desorption isotherm measurements to confirm the presence of GaN nanostructures. The nanorods are 6–7.5 nm in diameter, and can be a few hundreds of nm in length to exhibit nanowire structure. Freestanding GaN nanorod arrays were revealed upon removal of the silica framework with HF solution. Optical characterization of the isolated GaN nanorod arrays shows a strong and sharp near band-edge emission at 375 nm, and two phonon-assisted donor-acceptor peaks at 395 and 415 nm. A broad but weak emission in the region of 335–360 nm due to the quantum confinement effect of short nanorods was observed.

    TABLE OF CONTENTS Abstract i Acknowledgements ii Table of Contents iii List of Figures v List of Tables viii CHAPTER 1 SYNTHESIS AND CHARACTERIZATION OF NANOPARTICLES WITHIN MESOPOROUS SILICA 01 1.1 Introduction 01 1.2 Methods of Synthesis of Nanoparticles within Mesoporous Silica 02 1.2.1 Direct Addition of Metal Compounds in Sol-Gel Mixture 03 1.2.2 Impregnation with Metal Compounds Followed by Reduction, Thermolysis, or Other Treatment 04 1.2.3 Chemical Interaction of Metal Compounds with Functional Groups of Mesoporous Oxides 11 1.2.4 Chemical Vapor Deposition of Metal Compounds for Incorporation into Mesoporous Silica 14 1.2.5 Template Ion Exchange with Transition Metal Cations 17 1.2.6 Silica Casting over Metal-Containing Templates 19 1.3 Properties of Mesoporous Materials with Nanoparticles 25 1.3.1 Catalytic Properties 27 1.3.2 Optical Properties 30 1.4 Methods of Synthesis of Gallium Nitride Nanoparticles 36 1.4.1 Solid State Metathesis Reaction 36 1.4.2 Solvothermal Reaction 39 1.4.3 Quantum-Confined Gallium Nitride Nanostructures with Hard Templates 41 1.5 Summary 42 1.6 References 43 CHAPTER 2 FORMATION OF ARRAYS OF GALLLIUM NITRIDE NANORODS WITHIN MESOPOROUS SILICA SBA-15 51 2.1 Introduction 51 2.2 Experimental Section 52 2.3 Results and Discussion 54 2.4 Summary 70 2.5 References 71

    (1) Alivisatos, A. P. Science 1996, 271, 933.
    (2) Whitney, T. M.; Jing, J. S.; Searson, P. C.; Chien, C. L. Science 1993, 261, 1316.
    (3) Zhang, Z.; Ying, J. Y.; Dresselhaus, M. S. J. Mater. Res. 1998, 13, 1745.
    (4) Sasak, M.; Osada, M.; Sugimoto, N.; Inagaki, S.; Fukushima, Y. Micropor. Mesopor. Mater. 1998, 21, 597.
    (5) Yang, C.; Kalwei, M.; Schüth, F.; Chao, K., Appl. Catal. A: Gen. 2003, 254, 289.
    (6) Rioux, R. M.; Song, H.; Hoefelmeyer, J. D.; Yang, P.; Somorjai G. A. J. Phys. Chem. B 2005, 109, 2192.
    (7) Li, L.; Shi, J. L.; Yan, J. N. Chem. Commun. 2004, 1990.
    (8) Kim, S. W.; Son, S. U.; Lee, S. I.; Hyeon, T.; Chung, Y. K. J. Am. Chem. Soc. 2000, 122, 1550.
    (9) Kesanli, B.; Lin, W. Chem. Commun. 2004, 2284.
    (10) Parala, H.; Winkler, H.; Kolbe, M.; Wohlfart, A.; Fischer, R. A.; Schmechel, R.; Seggern, H. Adv. Mater. 2000, 12, 1050.
    (11) Winkler, H.; Birkner, A.; Hagen, V.; Wolf, I.; Schmechel, R.; Seggern, H.; Fischer, R. A. Adv. Mater. 1999, 11, 1444.
    (12) Zheng, S.; Gao, L.; Zhang, Q.; Zhang, W.; Guo, J. J. Mater. Chem. 2001, 11, 578.
    (13) Zhang, W. H.; Shi, J. L.; Chen, H. R.; Hua, Z. L.; Yan, D. S. Chem. Mater. 2000, 12, 1408.
    (14) Zhang, W. H.; Shi, J. L.; Chen, H. R.; Hua, Z. L.; Yan, D. S. Chem. Mater. 2001, 13, 648.
    (15) Wang, S. Z.; Choi, D.; Yang, S. M. Adv. Mater. 2002, 14, 1311.
    (16) Wellmann, H.; Rathousky, J.; Wark, M.; Zukal, A.; Ekloff, G. S. Micropor. Mesopor. Mater. 2001, 44/45, 419.
    (17) Xu, W.; Liao, Y.; Akins, D. L. J. Phys. Chem. B 2002, 106, 11127.
    (18) Besson, S.; Gacoin, T.; Ticholleau, C.; Jacquiod, C.; Boilt, J. Nano Lett. 2002, 2, 409.
    (19) Zhang, Z.; Dai, S.; Fan, X.; Blom, D. A.; Pennycook, S. J.; Wei, Y. J. Phys. Chem. B 2001, 105, 6755.
    (20) Shan, Y.; Gao, L. Mater. Chem. Phys. 2005, 89, 412.
    (21) Gao, F.; Lu, Q.; Zhao, D. Adv. Mater. 2003, 15, 739.
    (22) Srdanov, V. I.; Alxneit, I.; Stucky, G. D.; Reaves, C. M.; DenBaars, S. P. J. Phys. Chem. B 1998, 102, 3341.
    (23) Agger, J. R.; Anderson, M. W.; Remble, M. E.; Terasaki, O.; Nozue, Y. J. Phys. Chem. B 1998, 102, 3345.
    (24) Harwig, T.; Kellendonk, F. J. Solid State Chem. 1978, 24, 255.
    (25) Dai, L.; Chen, X. L.; Zhang, X. N.; Jin, A. Z.; Zhou, T.; Hu, B. Q.; Zhang, Z. J. Appl. Phys. 2002, 92, 1062.
    (26) Cheng, B.; Samulski, E. T. J. Mater. Chem. 2001, 11, 2901.
    (27) Shama, S.; Sunkara, M. K. J. Am. Chem. Soc. 2002, 124, 12288.
    (28) Ponce, F.A.; Bour, D.P. Nature 1997, 386, 351.
    (29) Someya , T.; Werner, R.; Forchel, A.; Catalano, M.; Cingolani, R.; Arakawa, Y. Science 1999, 285, 1905.
    (30) Bae, S. Y.; Seo, H.W.; Park, J.; Yang, H.; Kim, H.; Kim, S. Appl. Phys. Lett. 2003, 82, 4564.
    (31) Liang, C. H.; Meng, G.W.; Wang, G.Z.; Wang, Y.W.; Zhang, L. D.; Zhang, S.Y. Appl. Phys. Lett. 2001, 78, 3202.
    (32) Li, Y. X.; Trinchi, A.; Wlodarski, W.; Galatsis, K.; Kalantarzadeh, K. Sens. Actuators B 2003, 93, 431.
    (33) Fasol, G. Science 1996, 272, 1751.
    (34) Kim, H. M.; Kang, T. W.; Chung, K. S. Adv. Mater. 2003, 15, 567.
    (35) Nakamura, S. Science 1998, 281, 956.
    (36) Kocha, S. S.; Peterson, M. W.; Arent, D. J.; Redwing, J. M.; Tischler, M. A.; Turner, J. A. J. Electrochem. Soc. 1995, 142, L238.
    (37) Johnson, W. C.; Parsons, J. B.; Crew, M. C. J. Phys. Chem. 1932, 36, 2561.
    (38) Wu, Y.; Zhang, L.; Li, G.; Liang, C.; Huang, X.; Zhang, Y.; Song, G.; Jia, J.; Zhixiang, C. Mater. Res. Bull. 2001, 36, 253.
    (39) Mulukutla, R. S.; Asakura, K.; Kogure, T.; Namba, S.; Iwasawa, Y. Phys. Chem. Chem. Phys. 1999, 1, 2027.
    (40) Mulukutla, R. S.; Shidob, T.; Asakura, K.; Iwasawa, Y. Scripta Mater. 2001, 44, 1695.
    (41) Mulukutla, R. S.; Asakura, K.; Namba, S.; Iwasawa, Y. Chem. Commun. 1998, 1425.
    (42) Sun, T.; Ying, J. Y. Nature 1997, 389, 704.
    (43) Ying, J. Y.; Mehnert, C. P.; Wong, M. S. Angew. Chem. Int. Ed. 1999, 38, 56.
    (44) Plyuto, Y.; Berquer, J. M.; Jacquiod, C.; Ricolleau, C. Chem. Commun. 1999, 1653.
    (45) Froba, M.; Kohn, R.; Bouffaud, G. Chem. Mater. 1999, 11, 2858.
    (46) Weiping, C.; Lide, Z. J. Phys. Condens. Matter. 1997, 9, 7257.
    (47) Zheng, S.; Gao, L.; Zhang, Q.; Sun, J. J. Solid State Chem. 2001, 162, 138.
    (48) Chen, W.; Cai, W.; Wang, G.; Zhang, L. Appl. Surf. Sci. 2001, 174, 51
    (49) Chen, W.; Cai, W.; Zhang, L.; Wang, G.; Zhang, L. J. Colloid Interface Sci. 2001, 238, 291
    (50) Gedanken, A.; Tang, X.; Wang, Y.; Perkas, N.; Koltypin, Y.; Landau, M. V.; Vradman, L.; Herskowitz, M. Chem. Eur. J. 2001, 7, 4546
    (51) Liu, Z.; Terasaki, O.; Ohsuna, T.; Hiraga, K.; Shin, H. J.; Ryoo, R. ChemPhysChem 2001, 229.
    (52) Besson, S.; Gacoin, T.; Ricolleau, C.; Jacquiod, C.; Boilot, J. P. Nano Lett. 2001, 2, 409.
    (53) Liu, Z.; Sakamoto, Y.; Ohsuma, T.; Hirada, K.; Terasaki, O.; Ko, C. H.; Shin, H. J.; Ryoo, R. Angew. Chem. Int. Ed. 2000, 39, 3107.
    (54) Fukuoka, A.; Higashimoto, N.; Sakamoto, Y.; Sasaki, M.; Sugimoto, N.; Inagaki, S.; Fukushima, Y.; Ichikawa, M. Catal. Today 2001, 66, 23.
    (55) Huang, M. H.; Choudrey, A.; Yang, P. Chem. Commun. 2000, 1063.
    (56) Fukuoka, A.; Higashimoto, N.; Sakamoto, Y.; Inagaki, S.; Fukushima, Y.; Ichikawa, M. Micropor. Mesopor. Mater. 2001, 48, 171.
    (57) Shepard, D. S.; Mashmeyer, T.; Johnson, B. F. G.; Thomas, J. M.; Sankar, G.; Ozkaya, D.; Zhou, W.; Oldroyd, R. D.; Bell, R. C. Angew. Chem. Int. Ed. 1997, 36, 2242.
    (58) Zhou, W.; Thomas, J. M.; Shephard, D. S.; Johnson, B. F. G.; Ozkaya, D.; Maschmeyer, T.; Bell, R. G.; Ge, Q. Science 1998, 280, 705.
    (59) Joo, S. H.; Choi, S. J.; Oh, I.; Kwak, J.; Liu, Z.; Terasaki, O.; Ryoo, R. Nature 2001, 412, 169.
    (60) Moller, K.; Bein, T. Chem. Mater. 1998, 10, 2950.
    (61) Lebeau, B.; Fowler, C. E.; Mann, S.; Farcet, C.; Charleux, B.; Sanchez, C. J. Mater. Chem. 2000, 10, 2105.
    (62) Zhang, L.; Sun, T.; Ying, J. Y. Chem. Commun. 1999, 1103.
    (63) Hua, Z. L.; Shi, J. L.; Wang, L.; Zhang, W. H. J. Non-Cryst. Solids 2001, 292, 177.
    (64) Antochshunk, V.; Jaroniec, M. Chem. Commun. 1999, 2373.
    (65) Tanev, P. T.; Pinnavaia, T. J. Chem. Mater. 1996, 8, 2068.
    (66) Guari, Y.; Thieuleux, C.; Mehdi, A.; Reye, C.; Corriu, R. J. P.; Gallardo, S. G.; Phillipot, K.; Chaudret, B.; Dutartre, R. Chem. Commun. 2001, 1374.
    (67) Jung, J. S.; Chae, W. S.; McIntyre, R. A.; Seip, C. T.; Wiley, J. B.; O’Connor, C. J. Mater. Res. Bull. 1999, 34, 1353.
    (68) Morey, M. S.; Bryan, J. D.; Schartz, S.; Stucky, G. D. Chem. Mater. 2000, 12, 3435.
    (69) Bronstein, L. M.; Polarz, S.; Smarsly, B.; Antonietti, M. Adv. Mater. 2001, 13, 1333.
    (70) Dag, O.; Ozin, G. A.; Yang, H.; Reber, C.; Bussiere, G. Adv. Mater. 1999, 11, 474.
    (71) Mehnert, C. P.; Weaver, D. W.; Ying, J. Y. J. Am. Chem. Soc. 1998, 120, 12289.
    (72) Zhang, L.; Papaefthymiou, C.; Ying, J. Y. J. Phys. Chem. B 2001, 105, 7414.
    (73) MacLachlan, M. J.; Ginsburg, M.; Coombs, N.; Raju, N. P.; Greedan, J. E.; Ozin, G. A.; Manners, I. J. Am. Chem. Soc. 2000, 122, 3878.
    (74) Yonemitsu, M.; Tanaka, Y.; Ywamoto, M. Chem. Mater. 1997, 9, 2679.
    (75) Badiei, A. R.; Bonneviot, L. Inorg. Chem. 1998, 37, 4142.
    (76) Iwamoto, M.; Tanaka, Y. Catal. Surv. Jap. 2001, 5, 25.
    (77) Bronstein, L.; Krämer, E.; Berton, B.; Burger, C.; Förster, S.; Antonietti, M. Chem. Mater. 1999, 11, 1402.
    (78) Whilton, N. T.; Berton, B.; Bronstein, L.; Hentze, H. P.; Antonietti, M. Adv. Mater. 1999, 11, 1014.
    (79) Antonietti, M.; Groehn, F.; Hartmann, J.; Bronstein, L. Angew. Chem. Int. Ed. 1997, 36, 208.
    (80) Ortiz, R. V.; Larsen, G. Chem. Mater. 2002, 14, 858.
    (81) Zhao, M.; Sun, L.; Crooks, R. M. J. Am. Chem. Soc. 1998, 120, 7355.
    (82) Han, B. H.; Polarz, S.; Antonietti, M. Chem. Mater. 2001, 13, 3915.
    (83) Polarz, S.; Smarsly, B.; Bronstein, L.; Antonietti, M. Angew. Chem. Int. Ed. 2001, 40, 4417.
    (84) Corma, A.; Martinez, A.; Soria, V. M.; Monton, J. B. J. Catal. 1995, 153, 25.
    (85) Thomas, J. M.; Raja, R. Chem. Rec. 2001, 1, 448.
    (86) Raja, R.; Khimyak, T.; Thomas, J. M.; Hermans, S.; Johnson, B. F. G. Angew. Chem. Int. Ed. 2001, 40, 4638.
    (87) Okumura, M.; Nakamura, S.; Tsubota, S.; Nakamura, T.; Azuma, M.; Haruta, M. Catal. Lett. 1998, 51, 53.
    (88) Zhou, H.; Cai, W.; Zhang, L. Mat. Res. Bull. 1999, 34, 845.
    (89) Hirai, T.; Okubo, H.; Komasawa, I. J. Colloid Interface Sci. 2001, 235, 358.
    (90) Chan, R. W. Adv. Mater. 1990, 2, 314.
    (91) Munir, Z. A. Am. Ceram. Soc. Bull. 1988, 67, 342.
    (92) Yi, H. C.; Moore, J. J. J. Mater. Sci. 1990, 25, 1159.
    (93) Wallace, C. H.; Kim, S. H.; Rose, G. A.; Rao, L.; Heath, J. R. Appl. Phys. Lett. 1998, 72, 596.
    (94) Gaskell, D. R. Introduction to Metallurgical Thermodynamics, McGraw-Hill, New York 1973, p.26.
    (95) Holt, J. B.; Munir, Z. A. J. Mater. Sci. 1986, 21, 251.
    (96) Gillan, E. G.; Kaner, R. B. Chem. Mater. 1996, 8, 333.
    (97) Hu, J. Q.; Deng, B.; Zhang, W. X.; Tang, K. B.; Qian, Y. T. Chem. Phys. Lett. 2002, 351, 229.
    (98) Hwang, J. W.; Hanson, S. A.; Britton, D.; Evans, J. F.; Jensen, K. F.; Gladfelter, W. L. Chem. Mater. 1990, 2, 342.
    (99) Hwang, J. W.; Campbell, J. P.; Kozubowski, J.; Hanson, S. A.; Evans, J. F.; Gladfelter, W. L. Chem. Mater. 1995, 7, 517.
    (100) Janik, J. F.; Wells, R. L. Chem. Mater. 1996, 8, 2708.
    (101) Frank, A. C.; Fisher, R. A. Adv. Mater. 1998, 10, 961.
    (102) Frank, A. C.; Stowasser, F.; Miskys, C. R.; Ambacher, O.; Giersig, M.; Fisher, R. A. Phys. Stat. Sol. (a) 1998, 165, 239.
    (103) Rodewald, D.; Bill, J.; Beck, U.; Puchinger, M.; Wagner, T.; Greiner, A.; Aldinger, F. Adv. Mater. 1999, 11, 1502.
    (104) Wang, J.; Grocholl, L.; Gillan, E. G. Nano Lett. 2002, 2, 899.
    (105) Fischer, R. A.; Miehr, A.; Herdtweck, E.; Mattner, M. R.; Ambacher, O.; Metzger, T.; Born, E.; Weinkauf, S.; Pulham, C. R.; Parsons, S. Chem. Europ. J. 1996, 2, 1353.
    (106) Bill, J.; Aldinger, F.; Kienzle, A.; Riedel, R. German Patent 4430817 1994.
    (107) Riedel, R.; Greiner, A.; Miehe, G.; Dreßler, W.; Fueß, H.; Bill, J.; Aldinger, F. Angew. Chem. 1997, 109, 657. Angew. Chem. Int. Engl. 1997, 36603.
    (108) Weinmann, M.; Haug, R.; Bill, J.; Aldinger, F.; Schuhmacher, J.; Müller, K. J. Organomet. Chem. 1997, 541, 345.
    (109) Kher, S. S.; Wells, R. L. Chem. Mater. 1994, 6, 2056.
    (110) Xie, Y.; Qian, Y.; Wang, W.; Zhang, S.; Zhang, Y. Science 1996, 272, 1926.
    (111) Mićić, O. I.; Ahrenkiel, S. P.; Bertram, D.; Nozik, A. J. Appl. Phys. Lett. 1999, 75, 478.
    (112) Manz, A.; Birkner, A.; Kolbe, M.; Fischer, R. A. Adv. Mater. 2000, 12, 569.
    (113) Yamane, H.; Shimada, M.; DiSalvo, F. J. Mater. Lett. 2000, 42, 66.
    (114) Yamane, H.; Kajiwara, T.; Sekiguchi, T.; Shimada, M. Jpn. J. Appl. Phys. 2000, 39, L146.
    (115) Gillan, E. G.; Kaner, R. B. Inorg. Chem. 1994, 33, 5693.
    (116) Hector, A. L.; Parkin, I. P. Polyhedron 1995, 14, 913.
    (117) Grocholl, L.; Wang, J.; Gillan, E. G.. Chem. Mater. 2001, 13, 4290.
    (118) Sardar, K.; Rao, C. N. R. Adv. Mater. 2004, 16, 425.
    (119) Ozin, G. A.; Kuperman, A.; Stein, A. Angew. Chem. Int. Ed. Engl. 1989, 28, 359.
    (120) Stucky, G. D.; MacDougall, J. E. Science 1990, 247, 669.
    (121) Behrens, P.; Stucky, G. D. Angew. Chem. 1993, 105, 729.
    (122) Kelly, M. J. Adv. Mater. 1997, 9, 857.
    (123) Abe, T.; Tachibana, Y.; Uematsu, T.; Iwamoto, M. Chem. Commun. 1995, 1617.
    (124) Srdanov, V. I.; Alxneit, I.; Stucky, G. D.; Reaves, C. M.; DenBaars, S. P. J. Phys. Chem. B 1998, 102, 3341.
    (125) Agger, J. R.; Anderson, M. W.; Pemble, M. E.; Terasaki, O.; Nozue, Y. J. Phys. Chem. B 1998, 102, 3345.
    (126) Han, W.; Fan, S.; Li, Q.; Hu, Y. Science 1997, 277, 1287.
    (127) Fukuoka, A.; Araki, H.; Kimura, J. I.; Sakamoto, Y.; Higuchi, T.; Sugimoto, N.; Inagakic, S.; Ichikawa, M. J. Mater. Chem. 2004, 14, 752.

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