金屬硼矽酸鹽及鑭硼酸鹽的合成及鑑定

以作者查詢圖書館館藏

、以作者查詢臺灣博碩士

、以作者查詢全國書目

、勘誤回報

、線上人數：25

、訪客IP：3.23.101.82

姓名

張玲瑋(Ling-Wei Chang) 查詢紙本館藏

畢業系所

化學學系

論文名稱

金屬硼矽酸鹽及鑭硼酸鹽的合成及鑑定
(Syntheses and Characterization of Metal Borosilicates and a Lanthanum Borate)

相關論文

★ 探討有機鹼DBU與金屬salen錯合物在二氧化碳對環氧化物的環狀加成反應中的角色	★ 磷橋異核雙金屬錯合物的配位子移轉
★ 含有碳烯化合物之鈀金屬異相觸媒催化碳碳鍵生成反應之研究	★ 銅(I)催化的碳硫偶合反應中間產物研究
★ 鈾鍺酸鹽之合成與結構鑑定	★ 稀土元素配位聚合物和亞磷酸鹽之合成、晶體結構與發光性質研究
★ 含有機模板的錫鍺酸鹽與錫矽酸鹽之合成與其結構鑑定	★ 銅催化碳硫偶合反應之陽離子效應研究
★ 銅(I)催化碳-氮偶合反應之研究	★ 探討β芳香醚類斷裂之研究
★ 銅(I)催化碳-氮偶合反應之研究	★ 鋰鋁鈦磷酸鹽的合成、晶體結構及性質研究
★ 鋰鐵鈦磷酸鹽之晶體結構與離子導電度性質研究	★ 鈦磷酸鹽與鈦矽酸鹽之合成、晶體結構與性質研究
★ 有機-無機混成之金屬磷酸鹽/亞磷酸鹽骨架化合物的合成與性質研究	★ 極性溶劑對銅(I)催化碳-氮偶合反應之影響

檔案

[Endnote RIS 格式]

[Bibtex 格式]

[相關文章]

[文章引用]

[完整記錄]

[館藏目錄]

至系統瀏覽論文 ( 永不開放)

摘要(中)

本論文利用在封閉系統下的熔鹽法合成出Ba2[Si3B3O12(OH)] (A1)、Ba[Si2BO6(OH)] (A2) 及 β - LaB8O11(OH)5 (B) 三個化合物，以高溫高壓水熱法合成出Pb6Si8B2O25 (A3)。四個新穎結構的化合物皆藉由單晶 X 光繞射方法鑑定出化合物的晶體結構。化合物 A1 的空間群為中心對稱的 P21/n，為少見的三個單層結構所組成二維層狀結構，每個單層皆由 BO4 和 SiO4 四面體上的三個氧原子做為連接點形成63拓撲構成二維層狀結構，Ba2+座落於8圓環通道中與層與層之間。化合物 A2 的空間群為中心對稱的 P21/c，以4圓環和6圓環表示(42.62)(4.62)2拓撲形成曲折的單層之二維層狀結構，Ba2+座落於皺褶的凹處。化合物 A3 的空間群為中心對稱的 R3 ̅c，由12圓環形成雙層的(122)(123)2 拓撲，彼此共享氧原子連接形成二維層狀結構，其基礎建構單元(Fundamental Building Blocks, FBBs)為T8O23(T: B或Si)，以兩個(B(1)0.8Si(1)0.2)O4和六個(Si(2)0.933B(2)0.067)O4以氧原子共角連接形成，並以Si(3)O4四面體連接每個FBB形成雙層之二維層狀結構。化合物 B 的空間群為非中心對稱的 Pna21，FBB 為 [B8O13(OH)5]7-，可表示為4△4□：[ψ]<△2□>|<△2□>|<△2□>|□△，FBB 彼此共角連接形成二維的層狀結構，La3+位於9圓環通道中。本論文利用在封閉系統下熔鹽法及高溫高壓水熱法合成出四個新穎結構的化合物，並證明以此合成方法能合成出更多不同結構的材料。

摘要(英)

Four new compounds, Ba2[Si3B3O12(OH)] (A1) and Ba[Si2BO6(OH)] (A2), Pb6Si8B2O25 (A3) and β - LaB8O11(OH)5 (B), were synthesized by a flux growth method in a closed system and the high-temperature, high-pressure hydrothermal method. All crystal structures were characterized by single-crystal X-ray diffraction.
The space group of A1 is the centrosymmetric P21/n. Compound A1 contains planar slabs of borosilicate formed of tetrahedral building units which can be described as condensation of three 3-connected 2D single layers with a 63 network topology. The Ba2+ cations are located in both the interlayer and intralayer regions. The structure is unusual with respect to triple tetrahedral layers. The space group of A2 is the centrosymmetric P21/n. Compound A2 consists of very contorted (3,4)-connected single layers with the rare (42.62)(4.62)2 topology. Ba2+ cations are located in the cavities of the sheets. The space group of A3 is the centrosymmetric R3 ̅c. Compound A3 has a 2D layer structure with (122)(123)2 topology. The layer consists of a new fundamental building block (FBB) with the formula T8O23 (T: B or Si) formed by two (B(1)0.8Si(1)0.2)O4 tetrahedra and six (Si(2)0.933B(2)0.067)O4 tetrahedra. The space group of B is the noncentrosymmetric Pna21. Compound B consists of the FBB, [B8O13(OH)5]7-, with 4△4□：[ψ]<△2□>|<△2□>|<△2□>|□△. Each FBB shares oxygen atoms to formed 2D layer structure. The La2+ cations are located in 12-ring channels. The high-temperature, high-pressure hydrothermal method and the flux growth method in a closed system are versatile methods to synthesize new materialswith interesting properties.

關鍵字(中)

★ 硼矽酸鹽
★ 鑭硼酸鹽

關鍵字(英)

論文目次

摘要 i
Abstract ii
謝誌 iii
目錄 iv
圖目錄 viii
表目錄 xii
附錄之表目錄 xiii
第一章緒論 1
1-1 非線性光學 1
1-1-1 非線性光學晶體的原理 1
1-1-2 非線性光學晶體的材料設計及應用 3
1-2 硼矽酸鹽 9
1-2-1 硼矽酸鹽化合物 9
1-2-2 硼矽酸鹽非線性光學晶體 10
1-3 硼酸鹽 11
1-3-1 硼酸鹽的結構型態 11
1-3-2 陰離子基團理論 12
1-3-3 硼酸鹽非線性光學晶體 13
1-3-4 共邊硼酸鹽 15
1-4 研究動機 17
1-5 研究摘要 18
第二章實驗方法及儀器介紹 19
2-1 合成方法 19
2-1-1 高溫高壓水熱法 19
2-1-2 封閉系統下的熔鹽法 21
2-1-3 使用設備清單 22
2-1-4 使用藥品清單 22
2-2 鑑定方法 23
2-2-1 使用儀器列表 23
2-2-2 單晶X光繞射儀與結構分析 25
2-2-3 粉末X光繞射儀(PXRD) 31
2-2-4 X光能量散佈分析儀(EDS) 32
2-2-5 紅外線光譜儀(IR) 33
2-2-6 熱重-差示掃描量熱分析儀(TGA-DSC) 34
2-2-7 固態核磁共振光譜儀(SSNMR) 35
第三章結果與討論 37
3-1 實驗部分 37
3-1-1 Ba2[Si3B3O12(OH)] (A1)和Ba[Si2BO6(OH)] (A2)合成條件 37
3-1-2 Pb6Si8B2O25 (A3)合成條件 39
3-1-3 β - LaB8O11(OH)5 (B)合成條件 41
3-2 單晶X光繞射結構解析 42
3-2-1 單晶X光繞射分析 42
3-2-2 Ba2[Si3B3O12(OH)] (A1)結構解析 47
3-2-3 Ba[Si2BO6(OH)] (A2)結構解析 49
3-2-4 Pb6Si8B2O25 (A3)結構解析 51
3-2-5 β - LaB8O11(OH)5 (B)結構解析 53
3-3 結構描述與討論 56
3-3-1 Ba2[Si3B3O12(OH)] (A1)結構描述 57
3-3-2 Ba[Si2BO6(OH)] (A2)結構描述 61
3-3-3 Pb6Si8B2O25 (A3)結構描述 65
3-3-4 β - LaB8O11(OH)5 (B)結構描述 69
3-4 化合物鑑定與性質測量 74
3-4-1 Ba2[Si3B3O12(OH)] (A1)和Ba[Si2BO6(OH)] (A2)粉末X光繞射分析 74
3-4-2 Ba2[Si3B3O12(OH)] (A1) X光能量散佈光譜分析 76
3-4-3 Ba2[Si3B3O12(OH)] (A1)紅外線光譜分析 77
3-4-4 Ba2[Si3B3O12(OH)] (A1)熱重-差示掃描量熱分析 78
3-4-5 Ba2[Si3B3O12(OH)] (A1)的11B固態核磁共振分析 80
3-4-6 Ba2[Si3B3O12(OH)] (A1)的29Si固態核磁共振分析 82
3-4-7 Pb6Si8B2O25 (A3)粉末X光繞射分析 84
3-4-8 Pb6Si8B2O25 (A3) X光能量散佈光譜分析 85
3-4-9 Pb6Si8B2O25 (A3)紅外線光譜分析 86
3-4-10 Pb6Si8B2O25 (A3)熱重-差示掃描量熱分析 87
3-4-11 Pb6Si8B2O25 (A3)的11B固態核磁共振分析 89
3-4-12 Pb6Si8B2O25 (A3)的29Si固態核磁共振分析 92
3-4-13 β - LaB8O11(OH)5 (B)粉末X光繞射分析 94
第四章結論 95
參考文獻 97
附錄 103

參考文獻

1. Franken, e. P.; Hill, A. E.; Peters, C.; Weinreich, G., Phys. Rev. Lett., 1961, 7, 118.
2. Bragg, W. H.; Bragg, W. L., Proc. R. Soc. London, Ser. A, 1913, 88, 428-438.
3. Halasyamani, P. S.; Zhang, W. G., Inorg. Chem., 2017, 56, 12077-12085.
4. Roberts, D. A., IEEE J. Quantum Electron, 1992, 28, 2057-2074.
5. Montgomery, K. E.; Milanovich, F. P., J. Appl. Phys., 1990, 68, 3979-3982.
6. Zumsteg, F. C.; Bierlein, J. D.; Gier, T. E., J. Appl. Phys., 1976, 47, 4980-4985.
7. AIDONG, J.; Bochang, W.; CHUANGTIAN, C.; Guiming, Y., Scientia Sinica (Series B), 1983, 28, 235-243.
8. Kane, T. J.; Byer, R. L., Opt. Lett., 1985, 10, 65-67.
9. Chao, T.-L.; Chang, W.-J.; Wen, S.-H.; Lin, Y.-Q.; Chang, B.-C.; Lii, K.-H., J. Am. Chem. Soc., 2016, 138, 9061-9064.
10. Xue, D.; Betzler, K.; Hesse, H.; Lammers, D., Solid State Commun., 2000, 114, 21-25.
11. Liebau, F., Structural chemistry of silicates: structure, bonding, and classification. Springer Science & Business Media: 2012.
12. Strunz, H.; Nickel, E., 2001.
13. Krzhizhanovskaya, M.; Bubnova, R.; Filatov, S., J. Struct. Chem., 2014, 55, 1342-1355.
14. Stanley, C. J.; Jones, G. C.; Rumsey, M. S.; Blake, C.; Roberts, A. C.; Stirling, J. A.; Carpenter, G. J.; Whitfield, P. S.; Grice, J. D.; Lepage, Y., Eur. J. Mineral., 2007, 19, 575-580.
15. Parise, J.; Gier, T., Chem. Mater., 1992, 4, 1065-1067.
16. Zhou, Z.; Xu, X.; Fei, R.; Mao, J.; Sun, J., Acta Cryst. B72, 2016, 72, 194-200.
17. Zhou, Z.; Qiu, Y.; Liang, F.; Palatinus, L. s.; Poupon, M.; Yang, T.; Cong, R.; Lin, Z.; Sun, J., Chem. Mater., 2018, 30, 2203-2207.
18. Lu, Z.; Zhang, F.; Tudi, A.; Yu, S.; Yang, Z.; Pan, S., Inorg. Chem. Front., 2019, 6, 2200-2208.
19. Tang, R.-L.; Hu, C.-L.; Mao, F.-F.; Feng, J.-H.; Mao, J.-G., Chem. Sci., 2019, 10, 837-842.
20. Burns, P. C.; Grice, J. D.; Hawthorne, F. C., Can. Mineral., 1995, 33, 1131-1151.
21. Chen, C. T.; Wu, Y. C.; Li, R. K., Int. Rev. Phys. Chem., 1989, 8, 65-91.
22. Chen, C.; Wu, Y.; Jiang, A.; Wu, B.; You, G.; Li, R.; Lin, S., JOSA B, 1989, 6, 616-621.
23. Wu, Y.; Sasaki, T.; Nakai, S.; Yokotani, A.; Tang, H.; Chen, C., Appl. Phys. Lett., 1993, 62, 2614-2615.
24. Mori, Y.; Kuroda, I.; Nakajima, S.; Sasaki, T.; Nakai, S., Appl. Phys. Lett., 1995, 67, 1818-1820.
25. Wu, B.; Tang, D.; Ye, N.; Chen, C., Opt. Mater., 1996, 5, 105-109.
26. Chen, C.; Wang, Y.; Wu, B.; Wu, K.; Zeng, W.; Yu, L., Nature, 1995, 373, 322.
27. Peng, G.; Ye, N.; Lin, Z.; Kang, L.; Pan, S.; Zhang, M.; Lin, C.; Long, X.; Luo, M.; Chen, Y., Angew. Chem., 2018, 130, 9106-9110.
28. Mutailipu, M.; Zhang, M.; Wu, H.; Yang, Z.; Shen, Y.; Sun, J.; Pan, S., Nat. Commun., 2018, 9, 1-10.
29. Xia, M.; Jiang, X.; Lin, Z.; Li, R., J. Am. Chem. Soc., 2016, 138, 14190-14193.
30. Pauling, L., J. Am. Chem. Soc., 1929, 51, 1010-1026.
31. Huppertz, H., Z. Naturforsch., B, 2003, 58, 278-290.
32. Emme, H.; Huppertz, H., Chem. Eur. J., 2003, 9, 3623-3633.
33. Fuchs, B.; Heymann, G.; Wang, X.; Tudi, A.; Bayarjargal, L.; Siegel, R.; Schmutzler, A.; Senker, J.; Joachim‐Mrosko, B.; Saxer, A., Chem. Eur. J., 2020, 26, 6851.
34. Knyrim, J. S.; Roessner, F.; Jakob, S.; Johrendt, D.; Kinski, I.; Glaum, R.; Huppertz, H., Angew. Chem. Int. Ed., 2007, 46, 9097-9100.
35. Neumair, S. C.; Glaum, R.; Huppertz, H., Z. Naturforsch., B, 2009, 64, 883-890.
36. Neumair, S. C.; Kaindl, R.; Huppertz, H., J. Solid State Chem., 2012, 185, 1-9.
37. Neumair, S. C.; Knyrim, J. S.; Oeckler, O.; Glaum, R.; Kaindl, R.; Stalder, R.; Huppertz, H., Chem. Eur. J., 2010, 16, 13659-13670.
38. Wu, Y.; Yao, J.-Y.; Zhang, J.-X.; Fu, P.-Z.; Wu, Y.-C., Acta Crystallogr. Sect. Sect. E: Struct. Rep. Online, 2010, 66, i45-i45.
39. Chen, X.; Chen, Y.; Sun, C.; Chang, X.; Xiao, W., J. Alloys Compd., 2013, 568, 60-67.
40. Mutailipu, M.; Zhang, M.; Li, H.; Fan, X.; Yang, Z.; Jin, S.; Wang, G.; Pan, S., Chem. Commun., 2019, 55, 1295-1298.
41. Guo, F.; Han, J.; Cheng, S.; Yu, S.; Yang, Z.; Pan, S., Inorg. Chem., 2019, 58, 8237-8244.
42. Han, S.; Huang, C.; Tudi, A.; Hu, S.; Yang, Z.; Pan, S., Chem. Eur. J., 2019, 25, 11614-11619.
43. Jen, I.-H.; Lee, Y.-C.; Tsai, C.-E.; Lii, K.-H., Inorg. Chem., 2019, 58, 4085-4088.
44. Rabenau, A., Angew. Chem. Int. Ed., 1985, 24, 1026-1040.
45. Kennedy, G. C., Am. J. Sci., 1950, 248, 540-564.
46. Canfield, P. C.; Fisk, Z., Philos. Mag. B, 1992, 65, 1117-1123.
47. Cong, R. H.; Yang, T.; Li, H. M.; Liao, F. H.; Wang, Y. X.; Lin, J. H., Eur. J. Inorg. Chem., 2010, 2010, 1703-1709.
48. Friedrich, W.; Knipping, P.; Laue, M., Annalen der Physik, 1913, 346, 971-988.
49. A., P. R.; C., L. M. F., Structure Determination by X-Ray Crystallography. Springer: US, 1985.
50. Sheldrick, G. M., SHELXL-97., 1997.
51. Hartmann, S.; Hahn, E., Phys. Rev, 1962, 128, 2042.
52. Sheldrick, G. M. SAINT, Version 7.68A; Bruker/Siemens Area Detector Absorption Correction Program University of Göttingen, Germany, 2009.
53. Krause, L.; Herbst Irmer, R.; Sheldrick, G. M.; Stalke, D., J. Appl. Crystallogr., 2015, 48, 3-10.
54. Sheldrick, G. M. SHELXL-2017/1, Program for the Solution of Crystal Structures, University of Göttingen, Germany: 2017.
55. Cesbron, F., Mineralogical Magazine, 1987, 51, 471-472.
56. Little, M. A.; Ronson, T. K.; Hardie, M. J., Dalton Trans., 2011, 40, 12217-12227.
57. Gautam, C.; Yadav, A. K.; Singh, A. K., ISRN ceramics, 2012, 2012.
58. Shao, G.; Wu, X.; Kong, Y.; Cui, S.; Shen, X.; Jiao, C.; Jiao, J., Surf. Coat. Technol., 2015, 270, 154-163.
59. Van Wüllen, L.; Müller-Warmuth, W., Solid State Nucl. Magn. Reson., 1993, 2, 279-284.
60. Zhou, B.; Sun, W.; Zhao, B.-C.; Mi, J.-X.; Laskowski, R.; Terskikh, V.; Zhang, X.; Yang, L.; Botis, S. M.; Sherriff, B. L., Inorg. Chem., 2016, 55, 1970-1977.
61. Fyfe, C. A.; Skibsted, J.; Schwieger, W., Inorg. Chem., 2001, 40, 5906-5912.
62. Irwin, A.; Holmgren, J.; Jonas, J., Mater. Lett., 1987, 6, 25-30.
63. Magi, M.; Lippmaa, E.; Samoson, A.; Engelhardt, G.; Grimmer, A., J. Phys. Chem., 1984, 88, 1518-1522.
64. Walkley, B.; Provis, J., Mater. Adv., 2019, 1, 100007.

指導教授

李光華(Kwang-Hwa Lii)

審核日期

2021-7-19

推文