摘要
树枝状大分子(Dendrimer)是一类新型的功能高分子化合物,它们具有在分子水平上可以设计分子大小、形状和功能基团的独特性质。近年来,这类大分子的合成及其性质的研究不仅逐渐成为高分子领域的研究热点,而且在药物输送、催化剂、基因治疗及传感器等应用领域也取得了突破性的进展。所以,依据Dendrimer分子结构本身的特点,系统地开展分子功能化和应用方面的研究,致力解决传统领域的实际问题,是一个非常有前途的研究方向。
本论文由以下四部分内容组成:
1.我们以乙二胺为中心核,采用发散法通过Michael加成和酰胺化重复反应合成了一系列0.5~ 4.0代聚酰胺-胺型树状高分子PAMAM。通过红外光谱、核磁共振等手段对产品结构进行表征,并研究了PAMAM水溶液紫外可见光谱和荧光光谱。结果表明PAMAM树状高分子有很好的光学性能,在光学材料方面有广泛的应用前景。另外,我们采用荧光分光光度法研究了4.0代PAMAM树状分子与稀土金属Sm3+,Dy3+,Ce3+的络合作用。通过反应时间、PAMAM物质的量比、反应体系pH的条件选择试验,确定了PAMAM对Ce(III), Sm(III)及Dy(III)离子的最佳配位条件,该研究为制备尺寸可控的PAMAM树状高分子封闭的稀土原子簇提供了理论基础。
2.通过氯化钴、乙二醛和5.0代树状高分子反应合成了金属钴树状高分子配合物。并以亚甲基蓝为荧光探针,通过紫外-可见光谱、荧光光谱和同步荧光光谱法研究了金属钴树状高分子配合物与鲱鱼精DNA(hsDNA)的相互作用,并探讨了盐效应对它们的影响。结果表明,此配合物与hsDNA之间发生了静电相吸作用,NaCl不同程度抑制了配合物与hsDNA的结合。
3.通过共价自组装的方法制备了巯基丙酸单分子层修饰金电极,利用共价作用实现金属钴树状高分子固定化,制备成巯基丙酸/金属钴树状高分子修饰电极。将该传感器用于鸟嘌呤的催化氧化研究,探讨了溶液pH值、扫速速度、鸟嘌呤浓度等因素的影响。实验表明,该组装电极对鸟嘌呤具有很好的电催化氧化性能,并且降低了鸟嘌呤氧化电位。在pH=5.8的醋酸盐缓冲液中检测鸟嘌呤,检测限为6.6×10-7mol/L。
4.制备了树状高分子封装金/钯纳米粒子,然后掺杂壳聚糖修饰玻碳电极,利用表面氨基基团与DNA上的磷酸基团共价结合制备了新型DNA传感器,用循环伏安法和交流阻抗法进行表征,表明此方法增加了dsDNA在电极表面的固定量。并用此DNA传感器对蚕丝中丝胶抗氧化性的研究,结果发现丝胶有很好的抗氧化性能,当丝胶浓度为0.90 mg/mL时,清除羟基自由基的效果最好。
Dendrimer is a new type of functional macromolecule compound that have special characters of designing the molecular size, shape and functional group at the molecular level. Synthesis and properties of Dendrimer is becoming the focus gradually in the macromolecule field, recently. It also acquires a breakthrough in some application field, such as drug deliver, catalyst carrier, gene therapy, sensor etc. According to the characters of dendrimer structure, it is a very prospect research to study on the functionalization and application of molecular systematically and devoting to solving the practical problem in the traditional fields.
This thesis is composed of four parts, which are as follows:
1. A series of PAMAM dendrimers of 0.5~4.0 generation were synthesized by divergent method using ethylenediamine as a rawmaterial by means of Mickeal addition reaction and amidation reaction. Their structures were characterized by IR, NMR. Meanwhile their fluorescence and UV-Vis properties were studied. The results showed that PAMAM dendrimers have good optical property and wide prospect in the field of optical matericals. Also, the coordinations between Sm3+,Dy3+,Ce3+ and polyamidomine dendrimer were studied by the fluorescence spectrophotometric method. By experiments of reaction time, molar ratio of RE3+/PAMAM and pH value of solution, the best coordination conditions of rare earth ions (RE3+) and PAMAM were determined. These offer the theoretical foundation for the preparation of rare earth atom clusters, which were in the polyamidomine dendrimer and size controlled.
2. Cobalt (II) polyamidomine dendrimer was prepared by cobalt chloride, glyoxal and polyamidomine dendrimer 5.0 generation reacting. The interaction of cobalt(II) polyamidomine dendrimer complex with herring sperm (hsDNA) have been carried out using methylene blue (MB) as the probe molecule by absorption and fluorescence spectroscopy and synchronous fluorescence spectroscopy. And salt effect on their interaction was discussed. The results showed that the interaction of complex with hsDNA was electrostatic. The effect of sodium chloride showed that sodium ion can significantly constrain the interaction of complex with hsDNA.
3. A new chemically modified gold electrode was prepared by covalent self-assembled using 3-mercaptopropionic acid as a modifier, then 3-mercaptopropionic acid and cobalt (II) polyamidomine dendrimer modified electrode was prepared by the covalent interaction. The sensor can be used to study the electrocatalytic oxidation of guanine. The effects of pH value, scanning rate and guanine concentration were discussed. It showed that the assembled electrode has obvious electrocatalytic activity on guanine and decreased the oxidation potential of the guanine. The guanine was measured in acetate buffer solution (pH=5.8), the detection limit is 6.6×10-7mol/L.
4. Dendrimer encapsulated Au/Pd nanoparticles were prepared. The nanoparticles doping chitosan was modified on glass carbon electrode (GCE), and then a novel DNA sensor was prepared by a covalently action between amino group of electrode surface and phosphate group of DNA. The immobilization dsDNA was characterized by cyclic voltammetry and electrochemical impedance spectroscopy. Experiment results showed that the immobilized amount of DNA probe on modified layer increased. The DNA biosensor was adopted to study the antioxidant property of silk sericin. The results showed that sericin had very good antioxidant properties, scavenging·OH effect was the best when concentration of sericin was 0.90 mg/mL.
引文
陈华,朱良均,闵思佳,等.蚕丝丝胶蛋白的利用研究[J].东华大学报,2002, 28(3):132-136
程义云,陈大柱,何平笙.PAMAM分子与Cr3+离子配位作用的研究[J].功能高分子学报,2005(6):265-267.
丛日敏,罗运军,李国平,等. PAMAM树形分子与Cd2+的配位作用研究及CdS/PAMAM纳米复合材料的制备与表征[J].化学学报, 2005, 63(5), 421.
方惠群,于俊生,史坚.仪器分析[M].北京:科学出版社, 2001.311-319
顾微,周玉兰.生物材料聚酰胺-胺树状大分子在医学领域研究进展[J].高分子通报,2002, 4, 1-5.
郭茂林,杨频,杨斌盛,等.以溴化乙锭为荧光探针研究二氯二茂钛与DNA作用方式[J].科学通报, 1995, 40(13):1187.
韩巧荣.树状支化大分子的合成及其荧光性能研究[D].2001,西北师范大学,西安
韩巧荣,丁马太,夏海平.树状大分子的自组装表面修饰与荧光客体分子的相转移[J].功能材料,2006,12(37):1946-1948
蒋治良,李芳,李廷盛,等.共振散射光强度与金粒子粒径的关系[J].高等学校化学学报, 2000,21, 1488.
焦奎,杨涛,杨婕,等. DNA在Mg/聚2,6-吡啶二甲酸膜上的固定和杂交及其PAT基因片段的电化学阻抗谱测定[J].中国科学B辑:化学,2007, 7(1):36-42
李国平,罗运军,谭惠民.以树形分子为模板制备银纳米颗粒[J].化学学报, 2004, 62(12):1158
李国平,罗运军,徐厚才.树形分子保护下铜原子簇的制备[J].无机化学学报, 2004, 20(l):61
李国平,罗运军,徐才厚,等.银离子与聚酰胺-胺型树形高分子配位作用的研究[J].无机化学学报, 2003(11):1212-1215.
梁红波,魏焕郁,施文芳.树枝状聚醚酰胺基紫外光固化粉末涂料的研究[J].热固性树脂,2002,17(2):4-7
沈景山,孙丹丹,付连春,等.荧光光谱法研究抗癌药物与DNA的相互作用[J].光谱学与光谱分析, 2005,25(2):232.
盛家镛,林红,王磊,等.易溶性丝胶粉的微细结构及理化性能研究[J].丝绸,2000, 6:6-9
时伟杰,艾仕云,李金焕,等.基于树状高分子固定DNA的电化学生物传感器的研究[J].分析化学,2008, 3(36):335-338
孙伟,杨茂霞,钟江华,等.灿烂甲酚蓝在DNA修饰金电极上的电化学行为[J].物理化学学报, 2007,23(4):499-502
王冰冰,罗宇飞,贾欣茹,等.扇形PAMAM树枝状高分子的合成与表征[J].高分子学报, 2004, (2):304-308
王俊,陈红侠,于翠艳,等.树枝状聚酰胺-胺对O/W型模拟原油乳液的破乳性能[J].石油学报(石油加工), 2002, 18(3):60-64
王俊,杨锦宗,陈红侠,等.发散法合成树枝状高分子聚酰胺-胺[J].合成化学,2001,9(1):62-64
王金凤,贾欣茹,金钟,等.聚酰胺-胺型树枝状化合物与四氯化钛的配合及其催化作用初步研究[J].高等学校化学学报, 2001, 4(22):709-711
王金凤,贾欣茹,李盈,等.树枝状大分子的自组装超薄膜[J].高等学校化学学报, 2001,22(4):1773-1775
王金凤,贾欣如,金钟等.聚酰胺-胺型树枝状化合物与四氯化钛的配合及其催化作用初步研究[J].高等学校化学学报, 2001, 22(4): 709-711
王平红,张岐,王流芳,等.鬼臼酰肼镍(Ⅱ)金属配合物与DNA的相互作用[J].光谱学与光谱分析,2006,26(5):941
王燕铭,宋瑜,孔德领,等.光谱法研究聚酰胺-胺型树枝状高分子与DNA的相互作用[J].科学通报, 2005,50(13):1323
卫艳丽,董川.三种抗癌嘌呤类化合物与环糊精作用的研究[J].光谱学与光谱分析, 2004,24(7):862
徐厚才,罗运军,谭惠民,等.树形聚酰胺胺与Cu2+的络合作用[J].分析测试学报, 2001, 20(3):1-4
杨浩.三齿多吡啶钴(Ⅲ)、钌(Ⅱ)配合物的合成、表征及与DNA的相互作用[J].高等学校化学学报,2007,28(5):872.
杨岭,罗宇飞,贾欣茹,等. PAMAM树枝状高分子的自组装膜的微摩擦性能研究[J].高分子学报,2004,5:780-783
杨志旺.树枝状高分子金属络合物的合成及其催化性能研究[D].2002,西北师范大学,西安
叶玲,顾微,周玉兰.生物材料聚酰胺-胺树状大分子在医学领域研究进展[ J].高分子通报, 2002, (4 ): 1 -5.
章昌华,胡剑青,涂伟萍.聚酰胺胺(PAMAM)树状分子的合成[J].化工新型材料, 2005, 33(10): 32-34.
张雨青.丝胶蛋白的护肤、美容、营养和保健功能[J].纺织学报, 2002, 23(2):150-154
张志胜.树枝状大分子修饰的毛细管电色谱的制备与应用研究[D].北京化工大学,2005,北京
郑世昭,徐伟箭.聚酰胺-胺树形大分子的合成与应用[J].高分子通报, 2004(2): 81-84.
Abbaspour A, Mehrgardi M A. Electrocatalytic Oxidation of Guanine and DNA on a Carbon Paste Electrode Modified by Cobal Hexacyano- ferrate Films[J].Anal. Chem., 2004, 76:5690
Abbaspour A, Mehrgardi M A, Kia R. Electrocatalytic oxidation of guanine and ss-DNA at a cobalt(II) phthalocyanine modified Adsule S, Barve V, Chen D, Ahmed F, Dou Q P, Padhye S, Sarkar F H. Novel Schiff base copper complexes of quinoline-2 carboxaldehyde as proteasome inhibitors in human prostate cancer cells[J].J Med Chem,2006, 49(24):7242.
Aixue L, Fan Y, Ying M, Yang X R. Biosens. Electrochemical impedance detection of DNA hybridization based on dendrimer modified electrode[J]. Bioelectron, 2007, 22(8): 1716-1722
Alonso B, Armada P G, Losada J, et al. Amperometric enzyme electrodes for aerobic and anaerobic glucose monitoring prepared by glucose oxidase immobilized in mixed ferrocene-cobaltocenium dendrimers[J]. Biosensors bioelectronics, 2004,19:1617-1625
Astruc D, Chardac F. Dendritic Catalysts and Dendrimers in Catalysis[J]. Chem. Rev.,2001, 101(9): 2991.
Barron J A, Bernhard S, Houston P L, et al. Electroluminescence inRuthenium(Ⅱ)Dendrimers[J]. Phys. Chem. A., 2003,107: 8130-8133
Bielinska A U, Kukowska-Latallo J F, Johnson J. The interaction of plasmid DNA with polyamidoamine dendrimers: mechanism of complex formation and analysis of alterations induced in nuclease sensitivity and transcriptional activity of the complexed DNA[J].B BA-Biomembranes Ucleic Acids Res., 1997, 1353(2):180-188
Brett C M A, Brett A M O, Serrano S H P. On the adsorption and electrochemical oxidation of DNA at glassy carbon electrodes[J]. J. Electroanal. Chem., 1994,366 :225
Buhleier E,Wehner W, V?gtle F.“Cascade”-and“Nonskid-chain-like”Synth- eses of Molecular Cavity Topologies[J]. Synthesis, 1978, 155-158
Bustos E B, Jiménez M G G , Díaz-Sánchez B R, et al.Glassy carbon electrodes modified with composites of starburst-PAMAM dendrimers containing metal nanoparticles for amperometric detection of dopamine in urine[J]. Talanta , 2007,72: 1586–1592
Crooks R M, Zhao M Q, Sun L, et al. Dendrimer-Encapsulated Metal Nanoparticles: Synthesis, Characterization, and Applications to Catalysis [J]. Acc. Chem. Res., 2001,34(3): 181-190.
Cuadrado I, Moran M, Casado C M, et al. Ferrocenyl-functionalized poly(pro- pyleneimine) dendrimers[J]. J Organometallics, 1996,15:5278-5280
Cai X H, Rivas G., Farias P A M, et al. Evaluation of different carbon electrodes for adsorptive stripping analysis of nucleic acids[J]. Electroanalysis, 1996,8(8-9): 753-758
Caminade A M, Turrin C O, Sutra P, et al. Fluorinated dendrimers[J]. Current Opinion in Colloid and Interface Seience, 2003, 8:282~295
Cantor C, Schimmel P R. The Conformation of Biological Macromo- lecules[M], Freeman, San Francisco, Biophsical Chemistry, 1980,2:398
Chechik V, Zhao M Q, Crooks R M. Self-Assembled Inverted Micelles Prepared from a Dendrimer Template: Phase Transfer of Encapsulated Guests [J]. J. Am. Chem. Soc., 1999, 121: 4910-911.
Chung Y M, Rhee H K. Partial hydrogenation of 1,3-cyclooctadiene using dendrimer-encapsulated Pd–Rh bimetallic nano- particles[J]. Journal of Molecular Catalysis A: Chemical 2003,206: 291–298
Crooks R M, Zhao M, Sun L, et al. Dendrimer-Encapsulated MetalNanoparticles: Synthesis, Characterization, and Applications to Catalysis[J].Acc. Chem. Res., 2001,34(3):181-190.
Dabbousi B O, Rodrigue-Viejo J, Mukulec F V, et al. (Cdse)ZnS Core-Shell Quantum Dots: Synthesis and Characterization of a Size Series of Highly Lunescent Nanocrysllites[J]. J. Phys. Chem. B., 1997, 1016:9463-9475.
Dandliker P J, Diederich F, Gross M, et al. Dendritic prophyrins: Modulating redox potentials of electroactive chromophores with pendant multifunctionality[J]. Angew Chem Int Ed Engl, 1994, 33: 1739-1742.
Dandliker P J, Diederich F, Gross M, et al.Water-soluble Dendritic Porphrins: Synthetic Models of Globular Heme Proteins[J]. Angew. Chem., Tnt. Ed Engl., 1994, 33(23-24):2460
de Brabander-Van en Berg E M M, Meijer E W. Poly(propylene imine) Dendrimers: Large-Scale Synthesis by Hetereogeneously Catalyzed Hydrogenations[J]. Angew. Chem. , Int. Ed. Engl., 1993, 32(9):1308-1311
Dvronic P R, de Leuze-Jallouli A M, Owen M J, et al. Radially Layered Poly(amidoamine-organosilicon) Dendrimers[J]. Macro- molecules, 2000, 33(15):5366-5378.
Endo T, Yoshimura T, Esumi K.Synthesis and catalytic of gold-silver binary nanopartieles stabilized by PAMAM dendriminer[J]. J. Col. Int. Sci. 2005,286:602-609
Erica B B, Ma G G T, Blanca R D S, et al. Glassy carbon electrodes modified with composites of starburst-PAMAM dendrimers containing metal nanoparticles for amperometric detection of dopamine in urine [J]. Talanta, 2007, 72 (4): 1586-1592
Esumi K, Isono R, Yoshimura T. Preparation of PAMAM- and PPI- metal (Silver,Platinum,and Palladium) Nanocomposites and Their Cataytic Activities for Reduction of 4-Nitro- phenol[J].Langmuir, 2004, 20:237-243.
Esumi K, Akiyama S, Yoshimura T. Multilayer formation using oppositely charged gold and silver dendrimer nanocomposites[J]. Langmuir, 2003, 19:7679-7681
Esumi K, Kuwabara K, Chiba T, et al. Interaction between a hydrophobicallymodified Poly(amidoamine) dendrimer and surfactants in aqueous solutions [J].Collids and Surface,2002, 197:141-146.
Esumi K, Suzuki A, Yamahira A, et al. Role of poly(amidoamine) dendrimers for Preparing nanopartieles of gold,platinum,and silver[J]. Langmuir, 2000, 16:2604-2608
Fillaut J L, Linares J, Astruc D. Single-step six-electron transfer in a heptanuclear complex: Isolation of both redox forms[J]. Angew Chem Int Ed Engl, 1994, 33: 2460-2462.
Flory P J. Molecular Size Distribution in Three Dimensional Polymers. VI. Branched Polymers Containing A-R-Bf-1 Type Units[J]. J. Am. Chem.Soc.,1952,74(11):2718.
Frank N C, Emilia M G , Florescu M, et al. A strategy for enzyme immobili- zation on layer-by-layer dendrimer–gold nanoparticle electrocatalytic membrane incorporating redox mediator[J]. Electrochemistry Communications,2006, 8 :1665–1670
Fréchet J M J, Gitsov I, Grubbs R B, et al. New Approaches to Dendritic Macromolecules[J]. Polym. Mater. Sci. Eng.,1995,73:271-272
Garcia M E, Baker L A, Crooks R M. Preparation and charaeterization of dendrimer-gold colloid nanocomposites[J]. Analytical Chem.1999, 71(1):256-258
Gong A, Liu C, Chen Y, et al. A novel dendritic anion conductor: Quaternary ammonium salt of poly(amidoamine)(PAMAM)[J]. Macromol. Rapid Commun, 1999,20: 492-496
Goyal R N, Dryhurst G. Redox chemistry of guanine and 8-oxyguanine and a comparison of the peroxidase-catalyzed and electrochemical oxidation of 8-oxyguanine [J] J. Electroanal.Chem., 1994,369:253
Grabehev I, Bojinov V, Chovelon J M. Synthesis, Photophysical and Photochemical properties of fluorescent poly(amidoamine) dendrimers[J]. Polymer.2003,44:4421-4428
Grabchev I, Chovelon J-M, Bojinov V, et al. Poly(amidoamine) dendrimers Peripherally modified with 4-ethylamino-1,8–naphthalimide. Synthesis and Photophysical Properties[J]. Tetrahedron, 2003, 59: 9591-9598
Groot D de, Enunerink P G, Coueke C, et al. Rhodium catalysedhydroformylation using diphenylphosphine functionalized carbosilane dendrimers[J]. Inorg.Chem.Conunum., 2000,3: 711-13.
Haensler J, Szoka F C J. Polyamidoamine cascade polymers medite efficient Transfection of cells in culture[J]. Bioeonjug.Chem., 1993, 4(5):372-379.
Hawker C J, Fréchet J M J .A New Convergent Approach to Monodisperse Dendritic Macromoleeules[J]. J. Chem. Soc. Chem. Commun., 1990,15:1010-1013
Hawker C J, Wooley K L, Fréchet J M J. Solvatochromism as a Probe of theMicroenvironment in Dendritie Polyethers: Transition from an Extended to a Globular Structure[J]. J. Am. Chem. Soc.,1993,115(10):4375-4376
Hawker C J, Freehet J M J. Preparation of Polymers with Contorlled Molecular Architectuer. A New Convergent Approach to Dendritic Macromolecules[J]. J.Am.Chem.Soc. ,1990, 112: 7638-7647
Hawker C J, Fréchet J M J. Control of Surface Functionality in the Synthesis of Dendritic Macromolecules Using the Convergent- Growth Approach[J].Macromolecules,1990,23(21):4726
Hines M A, Guyot-Sionnest P. Synthesis and Characterization of Strongly Lumineseing ZnS-Capped Cdse Nanocrystals[J]. J.Phys.Chem,1996, l00(2):468-471.
Hong M Y, Yoon H C, Kim H S. Protein-ligand interactions at poly- (amidoamine) dendrimer monolayers on gold[J].Langmuir, 2003,19(2): 416-421.
Hu Z, Tong C L. Synchronous fluorescence determination of DNA based on the interaction between methylene blue and DNA[J].Analytica Chimica Acta ,2007 ,587 :187
Hudson R H E, Damha M J. Nucleic acid dendrimers: Novel biopolymer structures[J].J.Am.Chem.Soe.1993,115:2119-2124
Hudson R H E, Damha M J. Nucleic Acid Dendrimers: Novel Biopolymer Structures. J.Am.Chem.Soc., 1993,115(6): 2119-2124
Kawagachi T, Walker K L, W ilkins C L, et al. Double exponential dendrimer growth. J. Am. Chem. Soc, 1995, 117(8): 2159-2165.
Kazutake T, Héctor D A. Determination of solvation numbers of [RuII(bpy)3] and [RuII(tpy)2] functionalized-PAMAM dendri- mers adsorbed onto platinum electrode surfaces[J]. Electroanal. Chem, 2004, 567 (2): 249-256
Kim E, Kim K, Yang H, et al. Enzyme-amplified electrochemical detection of DNA using electrocatalysis of ferrocenyl-tethered dendrimer[J]. Anal. Chem, 2003, 75(21): 5665-5672
Kemr C V, Emma H A. DNA binding studies and site selective fluorecence sensitization of an anthryl probe[J].J Am Chem Soc, 1993,115:8547
Kojima C, Kono K, Mamyama K, et al. Synthesis of Polyamidomine Dendrimers Having Poly(Ethyleneglycol) Grafts and Ability to Encapsulate Anticancer Drugs[J]. Bioconjug Chem., 2000, 11(6): 910-917.
Korbut O, BuèkováM, Tarapèík P,et al.. Damage to DNA indi- cated by an electrically heated DNA-modified carbon paste electrode[J]. J. Electroanal Chem., 2001,506(2): 143-148
Krystyna A K, Angela F D N, Adolfo A C,et al. stability constants and structures of complexes of copper(II), nickel(II), silver(I) and mercury(II) with PAMAM dendrimer and related tetraamide ligands[J].Inorganica Chimica Acta, 2005, 358 (12):3497
Labuda J, BuèkováM, Mattusch J, et al. Voltammetric Detection of the DNA Interaction with Copper Complex Compounds and Damage to DNA[J]. Electroanalysis, 1999,11(2): 101-107
Lang H F, May R A, Iversen B L, et al. Dendrimer-Encapsulated Nanoparticle precursors to Supported Platinum Catalysts[J]. J. Am. Chem. Soc., 2003, 125(48):14832-14836.
Launay N, Caminade A M, Majoral J P. Synthesis and activity of Unusual Phosphorus Dendrimers. A Useful Diveent Growth Approach Up to the Seventh Generation. J. Am. Chem. Soc. , 1995,117(11): 3282-3283
Lemon B I, Crooks R M. Preparation and Characterization of Dendrimer-Encapsulated CdS Semiconductor Quantum Dots[J].J. Am. Chem. Soc., 2000,122:12886-12887.
Liu Z M, Yang Y, Wang H, et al. A hydrogen peroxide biosensor based on nano-Au/PAMAM dendriminer/Cystamine modified gold electrode [J].Sen. Act. B., 2005,106: 394-400
Lloyd D R , Phillips D H. Oxidative DNA damage mediated by copper (II), iron(II) and nickel (II) Fenton reactions: evid- ence for site- specific mechanisms in the formation of double-strand breaks, 8-hydro- deoxyguanosine and putative intrastarnd cross-links[J]. Mutation Research, 1999,424(1-2):23–36.
Long E C, Barton J K. On demonstrating DNA intercalation[J]. Acc.Chem. Res., 1990, 23(9):271.
Lun M S.AC Impedance Spectroscopy Principles and Applications[M] National Defence and Industry Press, Beijing, 2001.
Luo D, Haverstick K, Belcheva N, et al. Poly (ethylene glycol)-Conjugated PAMAM Dendrimer for Biocompatible, High- Efficiency DNA Delivery[J]. Macro- molecules.2002, 35(9): 3456
LuoY, Li Y, Jia X, et al. Fabrieation of Ag nanoparticle Encapsulating multilayer films based on pamam dendrimers with covalent interlayer1inkages[J].J. Appl. Polym. Sci.,2003,89:1515-1519
Marka A T G, John P H. Comparative Study of the Voltammetric Behaviour of Guanine at Carbon Paste and Glassy Carbon Electrodes and its Determination in Purine Mixtures by Differential-pulse Voltammetry[J]. Analyst, 1992,117(10): 1613
Marcos M, Omenat A, Serrano J L. Structure-mesomorphism relationship in terminally functionalised liquid crystal dendrimers[J]. Comptes Rendus Chimie, 2003, 6: 947-957.
Malik N R,Wiwattanapatapee R, Klopsch R, et al. Dendrimers: Relationship Between Structure and Biocompatibility in Vitro, and Preliminary Studies on the Biodistribution of Labelled Polyamidoamine Dendrimes in Vivo[J]. Journal of Controlled Release, 2000,65:133-148
Mello L D, Hernandez S,Marrazza G,et al.Investigations of the antioxidant properties of plant extracts using a DNA-electrochemical biosensor[J]. Biosensors and Bioelectronics , 2006, 21,1374–1382
Miller T M, Neenan T X, Zayas R, et al . Synthesis and characterization of a series of monodisperse, 1, 3, 5- phenylenebased hydrocarbon dendrimers including C276H1S6 and fluorinated analogues. J.Am. Chem. Soc , ,1992, 114: 1018-1025.
Miller T M, Neenan T X. Convergent Synthesis of Monodisperse Dendrimers Based Upon 1,3,5-trisubstituted Benzenes[J]. Chem. Mater., 1990, 2(4): 346-349
M?nica R P, Tania G, Encarnaci?n L,et al. Comprehensive study of interactions between DNA and new electroactive Schiff base ligands: Application to the detection of singly mismatched Helicobacter pylori sequences[J]. Biosensors and Bioelectronics, 2007, 22 (11):2675,
Newkome G R, Moorefield C N, Baker G. R, et al. Alkane cascade Polymersprocessing micellar topology: micellnaoic acid derivatives[J]. Angew. Chem. Int. Ed. Engl., 1991, 30: 1178-1180
Newkome G R, Yao Z Q, Baker G R, et al. Micelles. Part 1. Cascade molecules: a new approach to micelles. A [27]-arborol, J. Org.Chem., 1985,50(11): 2003-2004.
Newkome G R, Guther R, Moorefield C N, et al. Routes to dendritic networks: Bis-dendrimers by coupping of cascade macromolecules through metal centers[J]. Angew Chem Int Ed Engl, 1995, 34: 2023-2026.
Niu Y,Yeung L K,Crooks M. Size-Selective Hydrogenation of Olefins by Dendrirmer-Encapsulated Palladium Nanoparticles[J]. J.Am.Chem. Soe.,2001,123(28):6840-6846.
Ottavani M F, Montalt I F, Turro N J, et al. Characterization of starburst dendrimers by the EPR technique: Copper(Ⅱ) ions binding full_generation dendrimers[J]. J Phys Chem, B, 1997,101(2): 158-166.
Rebov E A, Muzafarov M, Papkov V S, et al. Dendritic Polyorganosilanes[J]. Dolk. Akad. Nauks. SSR ,1990,309:376
Rengan K, Engel R J. The Synthesis of Phosphonium Cascade[J].Molecules. J. Chem. Soc.,Perkin Ttans. , 1991, l: 987-990
Roberts J C, Bhalgat M K, Zara R T. Preliminary biological evaluation of polyamidoamine (PAMAM) Starburst Dendrimers[J]. J. Biomed. Mater. Res., 1996, (30): 53-65.
Sasaki M , Yamada H , Kato N. Consumption of silk protein, sericin elevates intestinal absorption of zinc , iron , magnesium and calcium in rats[J ] . Nutrition Research , 2000 , 20 (10) : 1505-1511.
Serroni S, Denci G, Gmapagaha S. Arborols from luminescent and redox-active transition metal Complex fragments. Angew. Chem. Int.Ed. Engl., 1992,31(11):1493-1495
Seyferth D, Son D Y, Rheingold A L, et al. Synthesis of an Organosilicon Dendrimer Containing 324 Si-H Bonds. Oranometallics, 1994, 13(7):2682-2690
Shukla S, Wu G, Ghatterjee M, et al.synthesis and Biological Evaluation ofFolate Receptor-Targeted Boronated PAMAM Dendrimers as Potential Agents for Neutron Capture Therapy[J]. Bioconjugate Chem., 2003,14(1):158-167.
Smith D K. Recent developments in dendrimer chemistry[J]. Tetrahedron. 2003,59:3797-3798
Stewart G M, Fox M A. Chromophore-Labeled Dendorns as Lihgt Harvesting Antennae[J]. J. Am.Chem.Soc.,1996,118: 4354-4360
Su C J, Liu Y C, Chen H L,et al.. Two-dimensional densely packed DNA nanostructure derived from DNA complexation with a low-generation poly(amidoamine) dendrimer[J]. Langmuir. 2007, 23(3): 975
Tomalia D A. Dendritic Macromolecules: Synthesis of Starburst Dendrimers Macromolecules. Macromolecules, 1986, 19(9):2466-2468
Tomalia D A, Baker H,Dewald J R,etal. A New Class of Polymers: Starburst-Dendritic Macromolecules. Polymer J. ,1985,17:117.
Tomalia D A, Dewald J R. Dense star polymer and dendrimers[P] US Patent, 4568737.1986
Tsukruk V V, Rinderspacher F, Bliznyuk V N. Self-assembled multilayer films from dendrimers[J]. Langmuir, 1997,13(8): 2171-2176
Uhrieh K E, Boegeman S, Fréchet J M J,et al. The solid-phase synthesis of dendritic polyamides. Polym. Bull.(Berlin). 1991, 25(5):551-558
Valerto C, Fillaut J L, Ruiz J, et al. The dendritic effect in molecular recognization: Ferrocene dendrimers and their use as
suppramolecular redox sensors for the recognition of small inorganic anions[J]. J Am Chem Soc, 1997, 119: 2588-2589.
Victor C, Ming Q Z, Crooks R M. Self-Assembled Inverted Micelles Prepared from a Dendrimer Template: Phase Transfer of Encapsulated Guests[J]. J. Am. Chem. Soc. 1999, 121, 4910-4911
V?gtle F, Gesteermann S, Hesse R, et al.Functional dendrimers. Prog. Polym. Sci. , 2000, 25:987-1041
Wang B D, Yang Z Y, Wang Q, et al. Synthesis, characterization, cytotoxic activities, and DNA-binding properties of the La(III) complex with Naringenin Schiff-base Bioorganic and Medicinal Chemistry, 2006,14:1880
Wang D, Kopeckova P, Minko T, et al. Synthesis of star-like Poly[N-(2-hydroxypropyl)methacrylamide) using PAMAM dendrimer as the core[J]. Polym Prepr, 2000, 41(1): 994.
Wang D, Kopeckova P, Minko T, et al. Synthesis of starlike N-(2-Hydroxypropyl)methacrylamide Copolymers: Potential Drug Carriers[J]. Biomacromolecules,2000,l(3):313-319
Wang J F, Jia X R, Zhong H, et al. Cinnamoyl Shell-modified Poly(amodoamine) Dendrimers[J]. J. Polym. Sci: Part A: Polym, Chem,2000,38:4147-4153.
Watanabe S, Regen S L. DendrimeRS as building block for multilayer construction[J].J. Am. Chem. Soe, 1994, 116: 8855 - 8856
Wang J, Jia X, Zhong H, et al. Cinnamoyl shell modified Poly(amidoamine) dendrimers[J]. J. Polym. Sci.,Polym.Chem. 2000,38: 4147-4153
Wang J, Bollo S, Lopez-Paz J L, et al. Ultratrace Measurements of Nucleic Acids by Baseline-Corrected Adsorptive Stripping Square-Wave Voltammetry[J]. Anal. Chem., 1999,71:1910
Wang J, Palecek E, Nielsen P E, et al. Peptide Nucleic Acid Probes for Sequence-Specific DNA Biosensors[J] J. Am. Chem. Soc. , 1996,118 :7667
Wells M, Crooks R M. Interactions between organized, surface-confined monolayers and vapor-phase probemolecules. 10. preparation and properties of chemically sensitive dendrimer surfaces [J]. J Am Chem Soc, 1996,118(16): 3988-3989
Wiener E C, Auteri F P, Chen J W, et al. Molecular dynamics of ion-chelate complexes attached to dendrimers[J]. J.Am. Chem.Soc.,1996, 118(33):7774-7782
Wooley K L, Hawker C J, Fréchet J M J. Dendrimers including C276H186 and theirFluorinated analogies. Angew. Chem. Int. Ed. Engl. 1994, 33:82-85
Wu X Y, Huang S W, Zhang T, et al. Preparation and Characterization ofNovel Physieally Cross-linked Hydrogels Composed of Poly(vinyl alcohol) and Amine-terminated Polyamidoamine Dendrimer[J]. Macromolecular Bioscience,2004, 24,4:71-75
Xu Y, Jiang Y, Fang Y Z, et al. Electrochemical impedance detec- tion of DNA hybridization based on the formation of M-DNA on polypyrrole/carbon nanotube modified electrode. Anal. Chim. Acta 2004, 516, 19-27.
Yoon H C, Kim H S. Multilayered assembly of dendrimerswith enzymes on gold: Thickness- controlled biosensing interface[J]. Analytical Chemistry. 2000, 72( 5):922- 926.
Yoon H C, Hong M Y , Kim H S. Functionulization of a poly-(amidoamine) dendrimer with ferrocenyls and its application to the construction of a reagentless enzyme electrode[J]. Analytical Chemistry, 2000, 72(18):4420-4427.
Yoon H C, Lee D, Kim H S. Reversible affinity interactions of antibody molecules at functionalized dendrimer monolayer: affinity- sensing surface with reusability [J].Analytica Chimica Acta,2002,(456): 209-218.
Zhang L, Huo F W, Wang Z Q, et al. Investigation into self -assembled monolayers of a polyether dendron thiol: chemisorption, kinetics, and patterned surfuace[J].Langmuir, 2000, 16(8): 3813-3817
Zhao M, Sun L, Crooks R M, et al .Hypebranched Polymer Film and Dendrmers[J].Polym Prepr., 1999, 40: 400-401.
Zhao M, Crook R M. Preparation of Cu nanoclusters within dendrimer templates[J].J Am Chem Soc, 1998,120:4877-4878.
Zhao M, Crook R M. Homogeneous hydrogenation catalysis with monodisperse, dendrimer-encapsulated Pd and Pt nano- particles[J]. Angew Chem Int Ed Engl. 1999,38:364-366.
Zhong X, Yi J, Sun J, et al. Synthesis an crystal structure of some transition metal complexe with a novel bis-Schiff base ligand and their antitumor activities[J]. Eur J Med Chem, 2006,41(9):1090.
Zhuo R X, Du B, Lu Z R. In vitro release of 5-fluorouracil with cyclic core dendritic Polymer[J]. J Controlled Rlease,1999, 57(3): 249-257.
