博碩士論文 982203021 詳細資訊




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:2 、訪客IP:3.145.64.235
姓名 廖英懿(In-yi Liao)  查詢紙本館藏   畢業系所 化學學系
論文名稱 雙核釕金屬錯合物之合成及其在染料敏化太陽能電池之應用
(New Ruthenium-Based Photosensitizers Incorporating Electron-Rich Cyclopentadienyl Ruthenium(II) Moiety for Dye Sensitized Solar Cells)
相關論文
★ 含胺基之二苯乙烯衍生物的分子內光誘導電子轉移之C-N斷鍵反應及激態錯合體之研究★ 含喹喔啉(quinoxaline)發色團的衍生物之光學性質與陰離子作用機構探討
★ 新型含1,2,3-三氮唑之雙光子吸收材料的合成及其光學性質探討★ 紫質衍生物研究:間位苯卟啉分子的鋅離子感測及大環紫質的構型
★ Squamocin 之合成研究★ 發展4,4’-亞甲基對苯胺或聯苯胺為骨架的四氯衍生物作為人類麩胺基硫轉移酶抑制劑的合成及構效關係的探討
★ 含有香豆素的石膽酸類似物作為唾液酸轉移酶抑制劑的合成與初步活性測試★ 石膽酸C4含氟唾液酸轉移酶抑制劑和苯並惡嗪酮相關的螢光探針之合成及生物研究
★ 合成和優化2-(1-乙基-3,5-二甲基-1H-吡唑-4-基)乙-1-胺衍生物和其抗三陰性乳腺癌細胞的體外活性研究★ 以蛋白質體學探討在大腸桿菌中甲醇利用代謝途徑
★ Data-independent acquisition mass spectrometry analysis for identification of cerebrospinal fluid biomarker of reversible cerebral vasoconstriction syndrome★ 從手性N-亞磺醯胺進行非對映選擇性磷酯基化反應建構高度選擇性的α-胺基磷酸酯
★ DNA型式碳水化合物抗原之生物偵測器的開發及應用★ 合成具有分子腳架之多並苯化合物且用於自組裝分子薄膜之研究
★ 1,3-偶極環化加成反應在藥物合成與醣晶片上的應用★ 平面化寡聚萘分子之合成及其光學、電學性 質研究
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]   [檢視]  [下載]
  1. 本電子論文使用權限為同意立即開放。
  2. 已達開放權限電子全文僅授權使用者為學術研究之目的,進行個人非營利性質之檢索、閱讀、列印。
  3. 請遵守中華民國著作權法之相關規定,切勿任意重製、散佈、改作、轉貼、播送,以免觸法。

摘要(中) 本論文中合成了一系列具有釕金屬以及環戊二烯作為多電子系統的有機金屬配位基,再以此配位基與釕金屬形成配位化合物。根據先前文獻指出具有多電子系統的釕金屬配位化合物其具有消光係數較大以及吸收光譜較紅位移的特點,而先前大多文獻在此方面多半以具有芳香環的胺類為多電子系統,但是具有胺類配位基的染料在氧化時容易產生自由基,使得染料趨於不穩定而產生變化,因此,我們利用具有穩定氧化還原的釕金屬化合物作為多電子的配位基,以改善有機配位基的缺點並承襲它在光譜上的優點,希望可以在染料敏化太陽能電池的應用上有更好的表現。
經元件測試結果,具釕金屬多電子系統之配位基之染料效率如下:Jsc = 3.08 mA/cm2、Voc = 0.53 V、FF = 0.66、??= 1.06%,效果明顯不如預期,這是因為LUMO能階與二氧化鈦導帶之能階差小於0.3 eV,因而電子注入二氧化鈦驅動式不足,使得光電流降低;其HOMO能階與電解質之氧化位能階差小於0.3 eV,因此二氧化鈦上的電子易與電解質競爭再生染料,使得光電壓降低。
摘要(英) We have synthesized a ruthenium(II)-polypyridyl photosensitizer, which contains an electron-rich cyclopentadienyl ruthenium (II) moiety in the polypyridyl ligand. The incorporation of electron-rich moiety in Ru(II)-based sensitizers has shown improvements in their extinction coefficients and bathochromic shift of the absorption spectral coverage. The photophysical properties and cell performance were studied in detail. The DSSC performance did not achieve the original expectation with efficiency 1.06% (Jsc = 3.08 mA/cm2, Voc = 0.53 V, FF = 0.66). The low photocurrent density was ascribed to the exist of low-lying LUMO level in CT-1, which lacks of sufficient driving force for charge injection. On the other hand, the exist of high-lying HOMO level resulted in rapid charge recombination that suppresses the open-circuit voltage to reach the expected value.
關鍵字(中) ★ 染料敏化太陽能電池
★ 釕金屬
關鍵字(英) ★ Ruthenium
★ Dye Sensitized Solar Cells
論文目次 中文摘要............................................... i
英文摘要............................................... ii
謝誌................................................... iii
圖目錄................................................. v
表目錄................................................. vi
第一章 緒論........................................... 1
1-1前言............................................... 1
1-2太陽能............................................. 2
?太陽能電池............................................ 5
1-3-1太陽能電池種類..................................... 6
矽晶片型太陽能電池....................................... 7
薄膜型太陽能電池......................................... 7
有機太陽能電池.......................................... 8
1-4 染料敏化太陽能電池 ( DSSC ).......................... 10
1-4-1 DSSC簡介........................................ 10
1-4-2 DSSC的運作機制.................................. 14
1-4-3 DSSC的效率計算.................................. 16
電流/電位曲線........................................... 17
短路電流............................................... 17
開路電壓............................................... 18
填充因子............................................... 18
效率計算............................................... 19
單色光光電轉換效率 (IPCE)................................ 19
1-4-4 DSSC的組成...................................... 20
透明導電陰極............................................ 20
半導體薄膜電極.......................................... 21
對電極................................................. 24
電解質................................................. 25
染料.................................................. 27
1-5 研究動機........................................... 42
第二章 實驗.......................................... 46
2-1 實驗儀器設備....................................... 46
2-2合成部份............................................ 50
第三章 結果與討論..................................... 67
3-1染料設計與合成....................................... 67
3-2 晶體特性........................................... 73
3-3 光物理性質......................................... 74
3-4 染料在二氧化鈦上的吸附情形............................ 77
3-5 染料之HOMO與LUMO能階................................ 78
3-6 DSSC元件效率....................................... 81
第四章 結論.......................................... 87
第五章 參考文獻....................................... 88
第六章 附錄.......................................... 92
參考文獻 1.BP Statistical Review of World Energy, June 2010.
2.(a) Hagfeldt A.; Boschloo, G.; Perrersson, Honrik.; Kloo, L.; Sun, L.C. Chem. Rev. 2010, 110, 6595-6663. (b) Service, R. F. Science 2005, 309, 548-550. (c) Potocnik, J. Science 2007, 315, 810-813. (d) Schiermeier, Q.; Tollefson, J.; Scully, T.; Witze, A.; Morton, O. Nature 2008, 454, 816-818.
3.Nelson, J. The Physics of Solar Cells; Imperial College Press: London, 2003.
4.Kim, H; Shin, M; Kim, Y. J. Phys. Chem. C, 2009, 113 , 1620–1623.
5.Gratzel, M. Nature 2001, 414, 338-344.
6.(a) Wronski, C. R. Conference Record of the 28th IEEE PhotoVoltaicSpecialists Conference, Anchorage, AK; IEEE: New York, 2000; p1.
7.(a) Repins, I.; Contreras, M.; Romero, M.; Yan, Y.; Metzger, W.; Li,J.; Johnston, S.; Egass, B.; DeHart, C.; Scharf, J.; MCandless, B. E.;Noufi, R. 2008.
8.(a) Shirakawa, H.; Chiang, C. K.; Fincher, C. R.; Park, Y. W.; Heeger, J. R.; Louis, E. J.; Gau, S. C.; MacDiarimd, A. G. Phys. Rev. Lett. 1977, 39. 1098-1107. (b)BoZano, L.; Carter, S. A.; Scott, J. C.; Malliaras, G. G.; Brock, P. J. Appl. Phys. Lett. 1999, 74, 1132 (c)Yu, G; Gao, J.; Hummele, J. C.; Widl, F.; Heeger, A. J. Science 1995, 270, 1789-1793. (d)Gunes, S.; Neugebauer, H.; Sariciftci, N. S. Chem. Rev, 2007, 107, 1324-1335. (e)Frohne, H; Shaheen, S.; Braec, C; Muller, D.; Saricidtci, N. S.; Meerholz, K. Chem. Phys. Chem. 2002, 9, 795-799. (f)Hoop, H.; Sariciftci, N. S. J. Mater. Chem. 2004, 19, 1924-30. (g)Eckert, J,–F.; Nicoud, J. –F.; Nierengarten, J. F.; Liu, S. –G.; Echegoyen, L.; Barigelletti, F.; Armaroli, N.; Ouali, L.; Karsnikov, V.; Hadziioannou, G. J. Am. Chem. Soc. 2000, 122, 7467-7474.
9.(a)劉顯杰,王世敏。有機染料敏化TiO2奈米經多孔膜液體太陽能電池研究進展。材料報導,2004, 18, 18-20. (b) Gratzel, M. Journal of Photobiology C:Photochemistry JP Review, 2003, 4, 145-153.
10.Hasselman, G. M.; Watson, D. F.; Stromberg, J. R.; Bocian, D. F.;Holten, D.; Lindsey, J. S.; Meyer, G. J. J. Phys. Chem. B 2006, 110, 25430-25442.
11.(a) Alonso, N.; Beley, M.; Chartier, P.; Ern, V. Appl Phys.Rev. 1981,16, 5. (c) Nimura, Y.; Amamiya, T; Tsubomura, H.; Matsumura, M. Nature 1976, 261, 402-403.
12.Desilvestro, J.; Gratzel, M.; Kavan, L.; Moser, J.; Augustynski, J. J. Am. Chem. Soc. 1985, 107, 2988-2993.
13.(a) Amadelli, R.; Argazzi, R.; Bignozzi, C. A.; Scandola, F. J. Am. Chem.Soc. 1990, 112, 7099-7103 (b) Nazeeruddin, M. K.; Liska, P.; Moser, J.; Vlachopoulos, N.; Grazel,M. Helv. Chim. Acta 1990, 73, 1788-1794.
14.Tennakone, K.; Kumara, G.; Kottegoda, I.; Wijayantha, K.; Perera, V. J. Phys. D: Appl. Phys. 1998, 31, 1492-1496.
15.Nazeeruddin, M. K.; Pechy, P; Renouard, T.; Zakeeruddin, S. M.; Baker, P. R.; Comte, P,; Liska, P.; Cevey, L.; Costa, E.; Shklover, V.; Spiccia, L,; Deacon, G. B.; Bignozzi, C. A.; Gratzel, M. J. Am. Chem. Soc. 2001, 123, 1613-1625.
16.Lindstrom, H.; Holmberg, A.; Magnusson, E.; Lindquist, S. E.; Malmqvist, L.; Hagfeldt, A., Nano Lett.2001, 1, 97-100.
17.(a) Hara, K.; Sayama, K.; Ohga, Y.; Shinpo, A.; Suga, S.; Arakawa,H. Chem.Commun. 2001, 569-570. (b) Hara, K.; Kurashige, M.; Dan-oh, Y.;Kasada, C.; Shinpo, A.; Suga, S.; Sayama, K.; Arakawa, H. New J. Chem. 2003, 27, 783-785.(c) Hara, K.; Sato, T.; Katoh, R.; Furube, A.; Ohga, Y.; Shinpo, A.; Suga, S.; Sayama, K.; Sugihara, H.; Arakawa H. J. Phys. Chem. B 2003, 107, 597-606.
18.Kitamura, T.; Hanabusa, K.; Wada, Y.; Yanagida, S,; Kubo, W., Chem. Commun. 2002, 374-375.
19.(a) O’Regan, B.; Gratzel, M. Nature. 1991, 353, 737-740. (b) Nazeeruddin, M. K.; Kay, A.; Rodicio, 1.; Baker, R. H.; Miiller, E.; Liska, P.; Vlachopoulos, N.; Gratzel. M. J. Am. Chem. Soc. 1993, 115, 6382. (c) Nazeeruddin, Md. K.; Zakeeruddin, S. M.; Baker, R. H.; Jirousek, M.; Liska, P.; Vlachopoulos, N.; Shklover, V.; Fischer, C. H.; Gratzel, M. Inorg. Chem. 1998. 38, 6298-6305.
20.Nazeeruddin, M. K.; Angelis, F. D.; Fantacci, S.; Selloni, A.; Viscardi, G.; Liska, P.; Ito, S.; Takeru, B.; Gratzel, M. J. Am. Chem. Soc. 2005, 127, 16835.
21.Nazeeruddin, M. K.; Pechy, P.; Renouard, T.; Zakeeruddin, S. M.; Baker, P. R.; Comte, P.; Liska, P.; Cevey, L.; Costa, E.; Shklover, V.; Spiccia, L.; Deacon, G. B.; Bignozzi, C. A.; Gratzel, M. J. Am. Chem. Soc. 2001, 123, 1613-17.
22.M. K. Nazeeruddin, F. D. Angelis, S. Fantacci, A. Selloni, G. Viscardi, P. Liska, S. Ito, B. Takeru, M. Gratzel, J. Am. Chem. Soc. 2005, 127, 16835-16842.
23.李言榮, 煇正中主編, 電子材料導論, 北京:清華大學出版社,2001. 34-96.
24.郝三存, 吳記懷, 林建明, 感光科學與光化學, 2004, 21 (3), 175-192.
25.康志敏, 郝彥忠, 王慶飛, 化學研究與應用, 2003, 15 (2), 32-87.
26.(a) Meng, Q. B.; Takahashi, K.; Zhang, X. T.; Sutanto, I.; Rao, T. N.; Sato, O.; Fujishima, A.; Watanabe, H.; Nakamori, T.; Uragami, M. Langmuir 2003, 19, 3572-3574. (b) Tennakone, K.; Kumara, G. R. R. A.; Kumarasinghe, A. R.; Wijayantha, K. G. U.; Sirimanne, P. M. Semicond. Sci. Technol. 1995, 10, 1689-1693. (c) Bach, U.; Lupo, D.; Comte, P.; Moser, J. E.; Weissortel, F.; Salbeck, J.; Spreitzer, H.; Gratzel, M. Nature 1998, 395, 583-585.
27.Horiuchi, T.; Miura, H.; Sumioka, K.; Uchida, S. J. Am. Chem. Soc. 2004, 126, 12218-12219. (b) Kuang, D; Uchida, S.; Humphry-Baker, R.; Zakeeruddin, S. M.; Gratzel, M. Angew. Chem. Int. Ed. 2008, 47, 1923-1927.
28.(a) Kim, D.; Lee, J. K.; Kang, S. O.; Ko, J. Tetrahedron 2007, 63, 1913-1922. (b) Wang, Z.-S.; Koumura, N.; Cui, Y.; Takahashi, M.; Sekiguchi, H.; Mori, A.; Kubo, T.; Furube, A.; Hara, K. Chem. Mater. 2008, 20, 3993-4003. (c) Zhang, X.-H; Wang, Z.-S.; Cui, Y.; Koumura, N.; Furube, A.; Hara, K. J. Phys. Chem. C 2009, 113, 13409-13415.
29. (a) Kim, S.; Lee, J. K.; Kang, S. O.; Ko, J.; Yum, J.-H.; Fantacci, S.; Angelis, F. D.; Censo, D. D.; Nazeeruddin, Md. K.; Gratzel, M. J. Am. Chem. Soc. 2006, 128, 16701-16707. (b) Kim, S.; Kim, D.; Choi, H.; Kang, M.-S.; Song K.; Kang S. O.; Ko, J. Chem. Commun. 2008, 4951-4953. (c) Choi, H.; Raabe, I.; Kim, D.; Teocoli, F.; Kim, C.; Song, K.; Yum, J.-H.; Ko, J.; Nazeeruddin, Md. K.; Gratzel M. Chem. Eur. J. 2010, 16, 1193-1201.
30.(a) Choi, H.; Lee, J. K.; Song, K. H.; Song, K.; Kanga, S. O.; Ko J. Tetrahedron 2007, 63, 1553-1559. (b) Choi, H.; Lee, J. W.; Song, K.; Kanga, S. O.; Ko, J. Tetrahedron 2007, 63, 3115-3121.
31.Tian, H.; Yang, X.; Pan, J.; Chen, R.; Liu, M.; Zhang, Q.; Hagfeldt, A.; Sun, L. Adv. Funct. Mater. 2008, 18, 3461-3468.
32.(a) Horiuchi, T.; Miura, H.; Sumioka, K.; Uchida, S. J. Am. Chem. Soc. 2004, 126, 12218-12219. (b) Kuang, D; Uchida, S.; Humphry-Baker, R.; Zakeeruddin, S. M.; Gratzel, M. Angew. Chem. Int. Ed. 2008, 47, 1923-1927.
33.(a) Hara, K.; Sayama, K.; Ohga, Y.; Shinpo, A.; Suga, S.; Arakawa, H. Chem. Commun. 2001, 569-570. (b) Hara, K.; Sato, T.; Katoh, R.; Furube, A.; Ohga, Y.; Shinpo, A.; Suga, S.; Sayama, K.; Sugihara, H.; Arakawa, H. J. Phys. Chem. B 2003, 107, 597-606. (c) Hara, K.; Kurashige, M.; Dan-oh, Y.; Kasad, C.; Shinpo, A.; Suga, S.; Sayama, K.; Arakawa, H. New J. Chem. 2003, 27, 783-785.
34. (a) Islam, A., Sugihara H., Singh L. P. Inorg. Chim. Acta 2001, 322, 7-16. (b) Islam A., Hara K., Singh L. P. Chem. Lett. 2000, 5, 490-491.
35. (a) Renouard T., Fallahpour R. A., Nazeeruddin M. K. Inorg. Chem. 2002, 41, 367-378. (b) Renouard T., Graetzel M. Tetrahedron, 2001 57, 8145-8150.
36. (a) Islam, A.; Sugihara, H.; Hara, K. J. Photochem. Photobiol. A: Chem. 2001, 145, 135-141.
37.Klein, C.; Nazeeruddin, M. K.; Liska P. Inorg. Chem., 2005, 44, 178-180.
38.(a)Klein, C.; Zazeeruddin, M. K.; Censo, D. Inorg. Chem. 2004, 43, 4216-4226. (b) Aranyos, V.; Hjelm, J.; Hagfeldt, A. J. Chem. Soc. Dalton. Trans., 2001: 1319-1325. (c) Aranyos, V.; Hjelm, J.; Hagfeldt, A. J. Chem. Soc., Dalton. Trans. 2003: 1280-1283.
39.Lagref, J. J.; Nazeeruddin, M. K.; Graetzel, M. Synth. Met., 2003, 138, 333-339
40.Wang, P.; Klein, C.; Baker, R. H. J. Am. Chem. Soc., 2005, 127, 808-809.
41.Hirate, N.; Durrant, J. R.; Nazeeruddin, M. K. Chem. Eur. J., 2004, 10, 595-602.
42.Johansson, O.; Borgstrom, M.; Lomoth, R. Inorg. Chem., 2003, 42, 2908-2918.
43.Ghanem, R.; Xu, Y.; Pan, J. Inorg. Chem., 2002, 41(24, 6258-6266.
44.(a) Chen, C.-Y.; Wu, S.-J.; Wu, C.-G.; Chen, J. G.; Ho, K.-C. Angew. Chem. Int. Ed. 2006, 45, 5822-5827. (b) Chen, C.-Y.; Lu, H.-C.; Wu, C.-G.; Chen, J.-G.; Ho, K.-C. Adv. Funct. Mater. 2007, 17, 29. (c) Chen, C.-Y.; Chen, J.-G. ;Wu, S.-J. Li,; J.-Y. Wu,; C.-G.; Ho, K.-C. (d) Chen, C.-Y.; Wang, M.; Li, J.-Y.; Pootrakulchote, N.; Alibabaei, L.; Ngocle, C.; Decoppet, J.-D.; Tsai, J.-H.; Gratzel, C. Wu, C.-G.; Zakeeruddin, S. M.; Gratzel, M. ACS Nano, 2009, 3, 3103-3109.
45.Jiang K. J., Masaki N., Xia J. Noda B., S., Yanagida S., Chem. Commun. 2006, 2460.
46.Robson K. C. D., Koivisto B. D., Gordon T. J., Baumgartner T., Berlinguette C. P. Inorg. Chem. 2010, 49, 5335-5337.
47.Bessho T., Yoneda E., Yum J.-H., Guglielmi M., Tavernelli I., Imai H, Rothlisberger U., Nazeeruddin M. K., Gratzel M. J. Am. Chem. Soc. 2008, 131 5930-5934.
48.Chang W.-C.; Chen H.-S.; Li T.-Y.; Hsu N.-M.; Tingare Y. S.; Li C.-Y.; Liu Y.-C.; Su C.; Li W.-R. Angew. Chem. 2010, 122, 8337 -8340.
49.Wu, K.-L.; Hsu, H.; Chen, K.; Chi, Y.; Chung, M.-W.; Liu, W.-H.; Chou, P.-T. Chem. Commun. 2010, 5124-5126.
50.Haque, S. A.; Handa, S.; Katja, P.; Palomares, E.; Thelakkat, M.; James, R. D. Angew. Chem. Int. Ed. 2005, 44, 5740 -5744.
51.Toyama, M.; Inoue, K.; Iwamatsu, S.; Nagao, N. Bull. Chem. Soc. Jpn. 2006, 79, 1525-1534.
52.Haberecht, M. C.; Schnorr, J. M.; Andreitchenko, E. V.; Clark, Jr.; Christopher, G.; Wagner, M.; Muellen K. Angew. Chem. Int. Ed. 2008, 47, 1662-1667.
53.Elliott, C. M.; Hershenhart, E. J. J. Am. Chem. Soc. 1982, 104, 7519-7526.
54.Shujiang, T.; Runhong, J.; Bo, J.; Junyong, Z.; Yan, Z.; Changsheng, Y.; Shunjun, J. Tetrahedron, 2007, 63, 381-388.
55.Yu, Z.; Najafabadi, H. M.; Xu, Y.; Nonomura, K.; Sun, L.; Kloo, L. Dalton Trans., 2011 , 40, 8361-8366.
56.Bruce M, I.; Ellis, B. G.; Low, P. J.; Skelton, B. W.; White A. H. Organometallics 2003, 22, 3184-3198.
57.Grosshenny, V.; Ziessel, R. J. Organomet. Chem., 1993 , 453, 2, 19-22.
58.Mann, J. R.; Gannon, M. K.; Fitzgibbons, T. C.; Detty, M. R.; Watson,D. F. J. Phys. Chem. C 2008, 112, 13057-13061.
59.童永樑, 工業材料雜誌 2008, 255, 109-113.
指導教授 孫世勝、侯敦仁
(Shih-Sheng Sun、Duen-Ren Hou)
審核日期 2012-1-24
推文 facebook   plurk   twitter   funp   google   live   udn   HD   myshare   reddit   netvibes   friend   youpush   delicious   baidu   
網路書籤 Google bookmarks   del.icio.us   hemidemi   myshare   

若有論文相關問題,請聯絡國立中央大學圖書館推廣服務組 TEL:(03)422-7151轉57407,或E-mail聯絡  - 隱私權政策聲明