在最後的實驗結果，我們發現到不同的萃取溫度、環境 pH 值與 PEG 分子量，對於萃取結果都會有所影響，隨著溫度的提升以及 PEG 分子量變大，下層相的銀奈米粒子會開始傾向分佈於上層相；而隨著 系統pH 值下降，上層相的銀奈米粒子會開始傾向分佈於下層相。我 們也找到理想的雙水相系統與萃取條件，來分離不同粒徑的銀奈米粒 子，在使用PEG 1500(20%)，K2HPO4(15%)，DI water(65%)的雙水相 系統，萃取溫度25℃，系統 pH 值 9，會有最佳的分離效果，此系統 直接進行三次批式萃取，經 SEM 偵測後，觀測到原本不均勻的銀奈 米粒子，會依不同尺寸而分離開來，且下層相都可以得到粒徑分佈較 小的小顆粒銀奈米粒子，因此使用雙水相系統簡單進行幾次批式萃取 後，的確可以成功分離不同粒徑大小的銀奈米粒子。
本研究的結果可以得到粒徑較一致的小顆粒銀奈米粒子，未來可 以嘗試使用不同鹽類或經過衍生化的 PEG 所組成的雙水相系統，來 分離得到粒徑較一致的大顆粒銀奈米粒子。
54
參考文獻
[1] S.B. Sinnotta, R. Andrewsb, "Carbon Nanotubes: Synthesis, Properties, and Applications". Critical Reviews in Solid State and Materials Sciences, 26 (2001) 145-249
[2] M.C. Daniel, D. Astruc, "Gold Nanoparticles: Assembly, Supramolecular Chemistry, Quantum-Size-Related Properties, and Applications toward Biology, Catalysis, and Nanotechnology".
Chem. Rev. 104 (2004) 293-346
[3] M.S. Yeh, Y.S. Yang, Y.P. Lee, H.F. Lee, Y.H. Yeh, C.S. Yeh,
"Formation and characteristics of Cu colloids from CuO powder by laser irradiation in 2-propanol". J. Phys. Chem. B 103 (1999) 6851-6857.
[4] Y. Kobayashi, A. Tomita, "Preparation of aqueous gold colloid by vapor deposition method". J. Colloid Interface Sci. 185 (1997) 285-286.
[5] M. Xu, C.R.H. Bahl, C. Frandsen, S. Morup, "Interparticle interactions in agglomerates of α-Fe2O3 nanoparticles: influence of grinding". J. Colloid Interface Sci. 279 (2004) 132-136
[6] Y. Chen, J.F. Gerald, J.S. Williams , S. Bulcock, "Synthesis of boron nitride nanotubes at low temperatures using reactive ball milling".
Chemical Physics Letters 299 (1999) 260–264
[7] L.L. Wang, J.S. Jiang, "Preparation of α-Fe2O3 nanoparticles by high-energy ball milling". Physica B 390 (2007) 23-27
[8] I. Lisiecki, M.P. Pileni, "Synthesis of copper metallic clusters using reverse micelles as microreactors". J. Am. Chem. Soc. 115 (1993) 3887-3896.
[9] A. Henglein, "Physicochemical properties of small metal particles in solution - microelectrode reactions, chemisorption, composite
55
metal particles, and the atom-to-metal transition". J. Phys. Chem.
97 (1993) 5457-5471.
[10] A.K. Nakamura, T. Sato, K. Sue, S. Tanaka, K. Saitoh, K. Aida, T.
Hiaki, "Rapid and continuous hydrothermal synthesis of metal and metal oxide nanoparticles with a microtube-reactor at 523 K and 30 MPa". Materials Letters 62 (2008) 3471-3473
[11] N. Murayama, N. Izu, W. Shin, I. Matsubara, "Preparation of SnO2 nanosized powder by precipitation method with nano-mixing of carbon powder". J. Ceram. Soc. Jpn. 113 (2005) 330-332.
[12] M.L. Wu, D.H. Chen, T.C. Huang, "Synthesis of Au/Pd bimetallic nanoparticles in reverse micelles". Langmuir 17 (2001) 3877-3883.
[13] M.T. Reetz, W. Helbig, "Size-selective synthesis of nanostructured transition-metal clusters". J. Am. Chem. Soc. 116 (1994) 7401-7402.
[14] N.V. Hullavarad, S.S. Hullavarad, "Synthesis and characterization of monodispersed CdS nanoparticles in SiO2 fibers by sol–gel method
". Photonics and Nanostructures – Fundamentals and Applications 5 (2007) 156-163
[15] S.F. Sweeney, G.H. Woehrle, J.E. Hutchison, "Rapid purification and size separation of gold nanoparticles via diafiltration". J. Am.
Chem. Soc. 128 (2006) 3190-3197.
[16] G. Tishchenko, K. Luetzow, J. Schauer, W. Albrecht, M. Bleha,
"Purification of polymer nanoparticles by diafiltration with polysulfone/hydrophilic polymer blend membranes". Sep. Purif.
Technol. 22-3 (2001) 403-415.
[17] X.Y. Xu, K.K. Caswell, E. Tucker, S. Kabisatpathy, K.L.
Brodhacker, W.A. Scrivens, "Size and shape separation of gold nanoparticles with preparative gel electrophoresis". J. Chromatogr.
A 1167 (2007) 35-41.
56
[18] M. Hanauer, S. Pierrat, I. Zins, A. Lotz, C. Sonnichsen, "Separation of nanoparticles by gel electrophoresis according to size-and shape". Nano Lett. 7 (2007) 2881-2885.
[19] D. Zanchet, C.M. Micheel, W.J. Parak, D. Gerion, S.C. Williams, A.P. Alivisatos, "Electrophoretic and structural studies of DNA-directed Au nanoparticle groupings". J. Phys. Chem. B 106 (2002) 11758-11763.
[20] P. Serwer, S.A. Khan, G.A. Griess, "Nondenaturing gel-electrophoresis of biological nanoparticles - viruses". J.
Chromatogr. A 698 (1995) 251-261.
[21] M.M.F. Choi, A.D. Douglas, R.W. Murray, "Ion-pair chromatographic separation of water-soluble gold monolayer-protected clusters". Anal. Chem. 78 (2006) 2779-2785.
[22] J. Stahlberg, "Retention models for ions in chromatography". J.
Chromatogr. A 855 (1999) 3-55.
[23] G.T. Wei, F.K. Liu, C.R.C. Wang, "Shape separation of nanometer gold particles by size-exclusion chromotography". Anal. Chem. 71 (1999) 2085-2091.
[24] G.T. Wei, F.K. Liu, "Separation of nanometer gold particles by size exclusion chromatography". J. Chromatogr. A 836 (1999) 253-260.
[25] T. Siebrands, M. Giersig, P. Mulvaney, C.H. Fischer, "Steric exclusion chromatography of nanometer-sized gold particles".
Langmuir 9 (1993) 2297-2300.
[26] J.P. Novak, C. Nickerson, S. Franzen, D.L. Feldheim, "Purification of molecularly bridged metal nanoparticle arrays by centrifugation and size exclusion chromatography". Anal. Chem. 73 (2001) 5758-5761.
[27] J.P. Wilcoxon, J.E. Martin, P. Provencio, "Size distributions of gold nanoclusters studied by liquid chromatography". Langmuir 16
57
(2000) 9912-9920.
[28] J.P. Wilcoxon, J.E. Martin, P. Provencio, "Optical properties of gold and silver nanoclusters investigated by liquid chromatography". J.
Chem. Phys. 115 (2001) 998-1008.
[29] C.A. Mirkin, R.L. Letsinger, R.C. Mucic, J.J. Storhoff, "A DNA-based method for rationally assembling nanoparticles into macroscopic materials". Nature 382 (1996) 607-609.
[30] R.C. Mucic, J.J. Storhoff, C.A. Mirkin, R.L. Letsinger, "One-Pot Colorimetric Differentiation of Polynucleotides with Single Base Imperfections Using Gold Nanoparticle Probes". J. Am. Chem. Soc.
120 (1998) 12674-12675.
[31] D.G. Thompson, A. Enright, K. Faulds, W.E. Smith, D. Graham,
"Ultrasensitive DNA Detection Using Oligonucleotide−Silver Nanoparticle Conjugates". Anal. Chem. 80 (2008) 2805-2810
[32] P.Å. Albertsson, "Partition of Cell Particles and Macromolecules in Polymer Two-Phase Systems". Advances in Protein Chem. 24 (1970) 309-341
[33] P.Å. Albertsson, "Partition of Cell Particles and Macromolecules
"3rd Ed, Wiley, 1986.
[34] F. Tjerneld, and D. Fisher, "Separations Using Aqueous Phase Systems". Plenum, 1989.
[35] Rajni Hatti-Kaul, "Aqueous Two-Phase Systems: Methods and Protocols: Methods and Protocols". Humana Press Inc., 2001
[36] J. Vernau, M.R. Kula, "Extraction of proteins from biological raw-material using aqueous polyethylene glycol-citrate phase systems". Biotechnol. Appl. Biochem. 12 (1990) 397-404.
[37] L.H.M. Silva, A.J.A. Meirelles, "PEG plus potassium phosphate plus urea aqueous two-phase systems: Phase equilibrium and protein
58
partitioning".J. Chem. Eng. Data 46 (2001) 251-255.
[38] R. Gupta, S. Bradoo, R.K. Saxena, "Aqueous two phase systems: an attractive technology for downstream processing of biomolecules".
Curr. Sci. 77 (1999) 520-523
[39] P.A.J. Rosa, A.M. Azevedo, I.F. Ferreira, J. de Vries, R. Korporaal, H.J. Verhoef , T.J. Visser , M.R. Aires-Barros, "Affinity partitioning of human antibodies in aqueous two-phase systems". J.
Chromatogr. A 1162 (2007) 103-113
[40] H.S.C. Barbosa, A.V. Hine, S. Brocchini, N.K.H. Slater, J.C. Marcos,
"Dual affinity method for plasmid DNA purification in aqueous two-phase systems". J. Chromatogr. A 1217 (2010) 1429-1436 [41] C.W. Ooi, B.T. Tey, S.L. Hii, S.M.M. Kamal, J.C.W. Lan, A. Ariff,
T.C. Ling, "Purification of lipase derived from Burkholderia pseudomallei with alcohol/salt-based aqueous two-phase systems".
Process Biochemistry 44 (2009) 1083-1087
[42] C.K. Su, B.H. Chiang, "Partitioning and purification of lysozyme from chickenegg white using aqueous two-phase system". Process Biochemistry 41 (2006) 257–263
[43] K.S. Jaw, L.H. Chou, S.M. Chang, K.J. Duan, "Purification of a trypsin inhibitor from sweet potato in an aqueous two phase system". Biotechnol Lett 29 (2007) 137-140
[44] G.D. Rodrigues, L.R. Lemos, L.H.M. Silva, M.C.H. Silva, L.A.
Minim, R. Coimbra, "A green and sensitive method to determine phenols in water and wastewater amples using an aqueous two-phase system". Talanta 80 (2010) 1139-1144
[45] V. Gonc﹐ A. Lacerda, A.B. Mageste, I.J.B. Santos, L.H.M. Silva, M.C.H. Silva, "Separation of Cd and Ni from Ni-Cd batteries by an environmentally safe methodology employing aqueous two-phase systems". Journal of Power Sources 193 (2009) 908-913
59
[46] C. W. Shen, T. Yu, "Size -fraction of silver nanoparticle using ion-pair extraction in a counter-current chromatography". J.
Chromatogr.A in press (2009).
[47] J. Zhang, J.R. Lakowicz, "Enhanced Luminescence of Phenyl-phenanthridine Dye on Aggregated Small Silver Nanoparticles". J. Phys. Chem. B 109 (2005) 8701-8706
[48] H.Y. Lin, C.T. Chen, Y.C. Chen, "Detection of phosphopeptides by localized surface plasma resonance of titania-coated gold nanoparticles immobilized on glass substrates". Anal. Chem. 78 (2006) 6873-6878.
[49] X. Lel, A.D. Dlamond, J.T. Hsu, "EquSkrium Phase Behavior of the Poly( ethylene glycol)/Potassium Phosphate/Water Two-Phase System at 4℃". J. Chem. Eng. Data 35 (1990) 420-423
[50] L.H.M. Silva, J.S.R. Coimbra, A.J.A. Meirelles, "Equilibrium Phase Behavior of Poly(ethylene glycol) + Potassium Phosphate + Water Two-Phase Systems at Various pH and Temperatures". J. Chem.
Eng. Data 42 (1997) 398-401
[51] U. Sivars, F. Tjerneld, "Mechanisms of phase behaviour and protein partitioning in detergent/polymer aqueous two-phase systems for purification of integral membrane proteins". Biochimica et Biophysica Acta 1474 (2000) 133-146
[52] S.Gautam, L. Simon, "Partitioning of B-glucosidase from Trichoderma reesei in poly(ethylene glycol) and potassium phosphate aqueous two-phase systems: Influence of pH and temperature". Biochemical Engineering Journal 30 (2006) 104–108 [53] D.P. Silva, M.Z. Pontes, M.A. Souza, M. Vitolo, J.B. Silva, A.P.
Junior, "Influence of pH on the partition of glucose-6-phosphate dehydrogenase and hexokinase in aqueous two-phase system".
Braz. J. Microbiol. 33 (2002) 196–201.
60
[54] S. Saravanana, J.R. Raoa, T. Murugesanb, B.U. Naira, T. Ramasami,
"Partition of tannerywastewater proteins in aqueous two-phase poly (ethylene glycol)-magnesium sulfate systems: Effects of molecular weights and pH". Chemical Engineering Science 62 (2007) 969-978