研究生: |
黃昱豪 Yu-Hao Huang |
---|---|
論文名稱: |
新穎的氮磷混合式配基的合成與錯合物之合成 Novel Hybrid N and P Ligands: Synthesis and Transition Metal Complexes |
指導教授: |
蔡易州
Yi-Chou Tsai |
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: | 中文 |
論文頁數: | 278 |
中文關鍵詞: | 混合式氮磷配基 |
外文關鍵詞: | hybrid N P ligand |
相關次數: | 點閱:1 下載:0 |
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氨氣是工業界及自然界極為重要的化合物,氮氣在地球上含量豐富,
且容易取得,利用它與適當的金屬催化劑反應產生氨氣是較具有經濟效益的方法。目前實驗室已經發展出一系列含氮磷的配基,分別為二芽基的N^P 配基與三芽基的N^P^N 配基,在N^P 配基方面:我們成功的與過渡金屬錳、鐵、鈷反應並純化得一系列的錯合物,並且利用X-ray 單晶繞射儀鑑定其結構。在N^P^N 配基方面:N^P^N 配基具有三種與金屬鍵結的模式,分別為中性的N^P^N 配基、帶負一價N^P^N 配基、帶負二價N^P^N配基,也利用了X-ray 單晶繞射儀成功的鑑定。此外,我們也將帶負一價N^P^N 配基與氯亞化鐵反應,並且順利純化出鐵錯合物。
Ammonia plays an important role in industry and nature.
Nitrogen is abundant and gained easily. It is more ommercial
benefit that using the nitrogen to mix with suitable metal-catalyst to create ammonia. We have developed a series of ligands that are hybridized by N and P. One of them is the N^P ligand that is bidentate and the other is the N^P^N ligand that is tridentate Presently, we have successfully prepared complexes M(N^P)(μ-Cl)2(Li)(THF)(Et2O) ( M = Mn、Fe、Co ) in good yields by treatment of one equivalent
of lithium salt of N^P ligand with a MCl2 .The complexes are
confirmed by X-ray single crystal diffraction. There are three binding modes of the N^P^N ligand binds to metal. It includes N^P^N、[N^P^N]Li、[N^P^N]Li2 .They are also identified by X-ray single crystal diffraction. Beside, we treat one equivalent of the [N^P^N]Li ligand with a FeCl2 and isolate iron(Ⅱ) complex successfully.
1.Fryzuk, M. D.; Johnson, S. A. Coordination Chemistry Reviews 2000,200–202, 379–409.
2.劉兆玄,科學月刊,1975 年10 月70 期
3.MacKay, B. A.; Fryzuk, M. D. Chem. Rev. 2004, 104, 385-401.
4.Odom, A. L.; Arnold, P. L.; Cummins, C. C. J. Am. Chem. Soc. 1998, 120, 5836-5837.
5.Smith, J. M.; Lachicotte, R. J.; Pittard, K. A.; Cundari, T. R.; Lukat-Rodfers, G.; Rodgers, K. R.; Holland, P. L. J. Am. Chem. Soc. 2001, 123, 9222-9223.
6.Howard, J. B.; Rees, D. C. Chem. Rev. 1996, 96, 2965-2982.
7.Christian, G.; Stranger, R. Dalton Trans. 2004, 2492-2495.
8.Cohen, J. D.; Fryzuk, M. D.; Loehr, T. M.; Mylvaganam, M.; Rettig S. J.Inorg. Chem. 1998, 37, 112-119.
9.Shaver, M. D.; Fryzuk, M. D. Adv. Synth. Catal. 2003, 345, 1061-1076.
10.(a) Cummins, C. C.; Baxter, S. M.; Wolczanski, P. T. J. Am. Chem. Soc.1988, 110, 8731-8733. (b) Schafer, D. F.; Wolczanski, P. T. J. Am. Chem. Soc. 1998, 120, 4881-4882.
11.Neithamer, D. R.; LaPointe, R. E.; Wheeler, R. A.; Richeson, D. S.; Van Duyne, G. D.; Wolczanski, P. T. J. Am. Chem. Soc. 1989, 111, 9056-9072.
12.Cummins, C. C. Chem. Commun., 1998, 1777-1786.
13.Odom, A. L.; Cummins, C. C.; Protasiewicz, J. D. J. Am. Chem. Soc. 1995, 117, 6613-6614.
14.Veige, A. S.; Slaughter, L. M.; Wolczanski, P. T.; Matsunaga, N.; Decker, S. A.; Cundari , T. R. J. Am. Chem. Soc. 2001, 123, 6419-6420.
15.Cao, Z.; Zhou, Z.; Wan, H.; Zhang, Q. Thiel, W. Inog. Chem. 2003, 42, 6986-6988.- 109 -
16.Eady, R. R. Chem. Rev. 1996, 96, 3013-3030.
17.Rod, T. H.; Nørskov, J. K. J. Am. Chem. Soc. 2000, 122, 12751-12763.
14.Fryzuk, M. D.; Love, J. B.; Rettig, S. J. Organometallics 1998, 17, 846-853.
15.Fryzuk, M. D.; Shaver, M. P.; Patrick, B. O. Inorganica Chimica Acta 2003, 350, 293-298.
16.Fryzuk, M. D.; Johnson, S. A.; Rettig, J. A. J. Am. Chem. Soc. 1998, 120, 11024-11025.
17.Schrock, R. R.; Seidel, S. W.; Schrodi, Y.; Davis, W. M. Organometallics 1999, 18, 428-437.
18.Hidai, M.; Mizobe, Y. Chem. Rev. 1995, 95, 1115-1133.
19.Six, C.; Beck, K.; Wegner, A.; Leitner, W. Organometallics 2000, 19, 4639-4642.
20.Guan, Z.; Marshall, W. J. Organometallics 2002, 21, 3580-3586.
21.(a) Smith, J. M.; Lachicotte, R. J.; Holland, P. L. Chem. Commun. 2001, 1542-1543. (b) Panda, A.; Stender, M.; Wright, R. J.; Olmstead, M. M.; Kelvins, P.; Power, P. P. Inorg. Chem. 2002, 41, 3909-3916.
22.Holland, P. L.; Cundari, T. R.; Perez, L. L.; Eckert, N. A.; Lachicotte, R. J. J. Am. Chem. Soc. 2002, 124, 14416-14424.
23.Fryzuk, M. D.; Love, J. B.; Rettig, S. J.Organometallics 1998, 17, 846-853.
24.Fryzuk, M. D.; Shaver, M. P.; Patrick, B. O. Inorganica Chimica Acta 2003, 350, 293-298.
25.Fryzuk, M. D.; Johnson, S. A.; Rettig, S. J. J. Am. Chem. Soc. 1998, 120, 11024-11025.
26.Fryzuk, M. D.; Carter, A.; Westerhaus, A. Inorg. Chem. 1985, 24, 642-648.
27.Schrock, R. R.; Seidel, S. W.; Schrodi, Y.; Davis, W. M.- 110 -
Organometallics 1999, 18, 428-437.
28.Fryzuk, M. D.; Yu, P.; Patrick, B. O. Can. J. Chem. 2001, 79, 1194-1200.
29.MacLachlan, E. A.; Fryzuk, M. D. Organometallics 2005, 24, 1112-1118.
30.Fryzuk, M. D.; Johnson, S. A.; Patrick, B. O.; Albinati, A.; Mason, S. A.; Koetzle, T. F. J. Am. Chem. Soc. 2001, 123, 3960-3973.
31.Fryzuka, M. D.; Petrellaa, M. J.; Coffina, R. C.; Patrickb, B. O. C. R. Chimie 2002, 5, 451-460.
32.Britovsek, G. J. P.; Gibson, V. C.; Wass, D. F. Angew. Chem. Int. Ed. 1999, 38, 428-447.
33.Ittel, S. D.; Johnson, L. K. Chem. Rev. 2000, 100, 1169-1203.
34.Gibson, V. C.; Spitzmesser, S. K. Chem. Rev. 2003, 103, 283-315.
35.Baumann, R.; Schrock, R. R.; Davis, W. M. J. Am. Chem. Soc. 1997, 119, 3830-3831.
36.Shaver, M. P.; Thomson, R. K.; Patrick, B. O.; Fryzuk, M. D. Can. J. Chem. 2003, 81, 1431-1437.
37.Bart, S. C.; Lobkovsky, E.; Chirik, P. J. J. Am. Chem. Soc. 2004, 126,13794-13807.
38.Smith, J. M.; Lachicotte, R. J.; Holland, P. L. Chem. Commun., 2001,1542–1543.
39.Kovacic, P.; Brace, N. O. J. Am. Chem. Soc. 1954, 76, 5491.
40.Budzelaar, H. M.; Oorta, A. B.; Orpenb, A. G. Eur. J. Inorg. Chem. 1998,1485-1494.
41.Tuczek, F.; Lehnert, N. Angew. Chem., Int. Ed. Engl. 1998, 37, 2636-2638.