HA/PDM自组装复合胶体粒子及其乳化性能

doi:10.3866/PKU.WHXB201302271

摘要/Abstract

摘要：

以阴离子天然大分子透明质酸(HA)和阳离子单体甲基丙烯酸二甲氨基乙酯(DM)组成带相反电荷的聚合物/单体复合体系, DM通过水相原位聚合可制备荷正电的聚甲基丙烯酸二甲氨基乙酯(PDM), PDM与HA间的静电作用可诱导两者在水溶液中进行自组装, 得到HA/PDM复合胶体粒子. 用傅里叶变换红外(FTIR)光谱仪对HA/PDM复合物结构进行了表征. 用动态激光光散射(DLS)研究了HA与PDM复合体系在水溶液中的自组装行为, 并表征了反应时间对HA/PDM复合胶体粒子粒径的影响. 利用透射电镜(TEM)表征了胶体粒子的形貌. 考察了溶液pH 对胶体粒子粒径及zeta 电位的影响, 并对胶体粒子的乳化性能进行初步探索. 结果表明:DM单体聚合前, 无HA/DM复合物聚集体形成; 而随着DM的逐步聚合, HA与PDM可通过静电作用逐渐组装形成球状HA/PDM复合胶体粒子, 其粒径随反应时间延长逐渐减小并趋于稳定. 同时, 该复合胶体粒子具有pH敏感性和乳化性, 乳化性能较纯HA和PDM有较大提高.

关键词: 透明质酸, 聚甲基丙烯酸二甲氨基乙酯, 静电作用, 自组装, 胶体粒子, 乳化

Abstract:

The anionic biomacromolecule, hyaluronic acid (HA), and cationic monomer, 2-(dimethylamino) ethyl methacrylate (DM), were used to construct an opposing charge polymer/monomer complex. Positively charged poly[2-(dimethylamino)ethyl methacrylate] (PDM) was prepared when DM monomers polymerized in aqueous solution. Self-assembly between PDM and HA was driven by electrostatic interaction, and HA/PDM complex colloid particles were formed in the aqueous medium. The HA/PDM complex structure was characterized by Fourier transform-infrared (FTIR) spectroscopy. The self-assembly behavior between HA and PDM, and the influence of polymerization time on HA/PDM complex colloid particle size, were investigated by dynamic laser scattering (DLS). Morphologies of the colloid particles were characterized by transmission electron microscopy (TEM). The influence of pH on the size and zeta potential of the colloid particles was investigated, and the emulsification of the colloid particles was preliminarily explored. The results showed that no HA/DM complex aggregates were formed before the polymerization of DM monomers. Spherical HA/PDM particles were spontaneously formed through electrostatic interaction between HA and PDM, coinciding with the gradual polymerization of DM. Particle sizes gradually decreased and stabilized with increasing polymerization time. The HA/PDM particles were pH sensitive and possessed improved emulsification properties compared with uncomplexed HA and PDM.

Key words: Hyaluronic acid, Poly[2-(dimethylamino)ethyl methacrylate], Electrostatic interaction, Self-assembly, Colloid particle, Emulsification

王娟勤, 白绘宇, 易成林, 刘娜, 刘晓亚. HA/PDM自组装复合胶体粒子及其乳化性能[J]. 物理化学学报, 2013, 29(05), 1028-1034. doi: 10.3866/PKU.WHXB201302271

WANG Juan-Qin, BAI Hui-Yu, YI Cheng-Lin, LIU Na, LIU Xiao-Ya. Self-Assembled HA/PDM Particles and Emulsification Properties[J]. Acta Phys. -Chim. Sin. 2013, 29(05), 1028-1034. doi: 10.3866/PKU.WHXB201302271

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201302271

https://www.whxb.pku.edu.cn/CN/Y2013/V29/I05/1028

参考文献

(1) Kötz, J.; Kosmella, S.; Beitz, T. Prog. Polym. Sci. 2001, 26 (8),1199. doi: 10.1016/S0079-6700(01)00016-8
(2) Zintchenko, A.; Dautzenberg, H.; Tauer, K.; Khrenov, V.Langmuir 2002, 18 (4), 1386. doi: 10.1021/la011267u
(3) Dautzenberg, H. Macromolecules 1997, 30 (25), 7810.doi: 10.1021/ma970803f
(4) Kamimura, M.; Kim, J. O.; Kabanov, A. V.; Bronich, T. K.;Nagasaki, Y. J. Control. Release 2012, 160 (3), 486. doi: 10.1016/j.jconrel.2012.04.027
(5) Harada, A.; Kataoka, K. Science 1999, 283 (5398), 65. doi: 10.1126/science.283.5398.65
(6) Cheng, Z. Y.; Ren, B. Y.; Gao, M.; Liu, X. X.; Tong, Z.Macromolecules 2007, 40 (21), 7638. doi: 10.1021/ma071072e
(7) Liu, Z. H.; Shang, Y. Z.; Huang, Y. M.; Peng, C. J.; Liu, H. L.Acta Phys. -Chim. Sin. 2011, 27 (5), 1135. [刘振海, 尚亚卓,黄永民, 彭昌军, 刘洪来. 物理化学学报, 2011, 27 (5), 1135.]doi: 10.3866/PKU.WHXB20110406
(8) Morfin, I.; Buhler, E.; Cousin, F.; Grillo, I.; Boué, F.Biomacromolecules 2011, 12 (4), 859. doi: 10.1021/bm100861g
(9) De la Fuente, M.; Seijo, B.; Alonso, M. J. Macromol. Biosci.2008, 8 (5), 441.
(10) Cai, H.; Ni, C. H.; Zhang, L. P. Eur. J. Pharm. Sci. 2012, 45 (1-2), 43. doi: 10.1016/j.ejps.2011.10.020
(11) Yang, J. S.; Chen, S. B.; Fang, Y. Carbohyd. Polym. 2009, 75 (2), 333. doi: 10.1016/j.carbpol.2008.07.037
(12) Boddohi, S.; Moore, N.; Johnson, P. A.; Kipper, M. J.Biomacromolecules 2009, 10 (6), 1402. doi: 10.1021/bm801513e
(13) Hu, Y.; Jiang, X. Q.; Ding, Y.; Chen, Q.; Yang, C. Z. Adv. Mater.2004, 16 (11), 934.
(14) Ding, Y.; Chen, Q.; Qian, H. Q.; Chen, Y.;Wu,W.; Hu, Y.;Jiang, X. Q. Macromol. Biosci. 2009, 9 (12), 1272. doi: 10.1002/mabi.v9:12
(15) Hu, Y.; Chen, Y.; Chen, Q.; Zhang, L. Y.; Jiang, X. Q.; Yang, C.Z. Polymer 2005, 46 (26), 12703. doi: 10.1016/j.polymer.2005.10.110
(16) Guo, R.; Zhang, L. Y.; Jiang, Z. P.; Cao, Y.; Ding, Y.; Jiang, X.Q. Biomacromolecules 2007, 8 (3), 843. doi: 10.1021/bm060906i
(17) Gatej, I.; Popa, M.; Rinaudo, M. Biomacromolecules 2005, 6 (1), 61. doi: 10.1021/bm040050m
(18) Lee, H.; Lee, K.; Park, T. G. Bioconjugate Chem. 2008, 19 (6),1319. doi: 10.1021/bc8000485
(19) Tanaka, N.; Yoshiike, Y.; Yoshiyama, C.; Kitaoka, T. Carbohyd.Polym. 2010, 82 (1), 100. doi: 10.1016/j.carbpol.2010.04.028
(20) Xu, J.; Ai, L.; Bai, H. Y.; Jiang, J. Q.; Xia,W. S.; Liu, X. Y.Polymer Bulletin 2011, No. 2, 78. [徐晶, 艾玲, 白绘宇,江金强, 夏文水, 刘晓亚. 高分子通报, 2011, No. 2, 78.]
(21) Lenormand, H.; Deschrevel, B.; Vincent, J. Carbohyd. Polym.2010, 82 (3), 887. doi: 10.1016/j.carbpol.2010.06.011
(22) Xu, J.; Bai, H. Y.; Yi, C. L.; Luo, J.; Yang, C.; Xia,W. S.; Liu,X. Y. Carbohyd. Polym. 2011, 86 (2), 678. doi: 10.1016/j.carbpol.2011.05.006
(23) Tao, Y. H.; Xu, J.; Chen, M. Q.; Bai, H. Y.; Liu, X. Y. Carbohyd.Polym. 2012, 88 (1), 118. doi: 10.1016/j.carbpol.2011.11.075
(24) Tan, Y.; Xu, K.; Liu, C.; Li, Y.; Lu, C.;Wang, P. Carbohyd.Polym. 2012, 88 (4), 1358. doi: 10.1016/j.carbpol.2012.02.018
(25) Yusoff, A.; Murray, B. S. Food Hydrocolloids 2011, 25 (1), 42.doi: 10.1016/j.foodhyd.2010.05.004
(26) Gharsallaoui, A.; Yamauchi, K.; Chambin, O.; Cases, E.; Saurel,R. Carbohyd. Polym. 2010, 80 (3), 820.
(27) Tømmeraas, K.; Mellergaard, M.; Malle, B. M.; Skagerlind, P.Carbohyd. Polym. 2011, 85 (1), 178.
(28) Van deWetering, P.; Zuidam, N. J.; Van Steenbergen, M. J.; Vander Houwen, O. A. G. J.; Underberg,W. J. M.; Hennink,W. E.Macromolecules 1998, 31 (23), 8065.
(29) Wu, Y.; Guo, J.; Yang,W. L.;Wang, C. C.; Fu, S. K. Polymer2006, 47 (15), 5289.
(30) Zhao, Y. Q.; Fei, F.; Yi, C. L.; Jiang, J. Q.; Luo, J.; Liu, X. Y.Acta Phys. -Chim. Sin. 2010, 26 (12), 3233. [赵艳琼, 费凡,易成林, 江金强, 罗静, 刘晓亚. 物理化学学报, 2010, 26
(12), 3233.] doi: 10.3866/PKU.WHXB20101217
(31) Cowman, M. K.; Matsuoka, S. Carbohyd. Res. 2005, 340 (5),805.
(32) Akiyama, E.; Kashimoto, A.; Fukuda, K.; Hotta, H.; Suzuki, T.;Kitsuki, T. J. Colloid Interface Sci. 2005, 282 (2), 452.
(33) Zinoviadou, K. G.; Scholten, E.; Moschakis, T.; Biliaderis, C. G.Int. Dairy J. 2012, 26 (1), 98.
(34) Amalvy, J. I.; Armes, S. P.; Binks, B. P.; Rodrigues, J. A.; Unali,G. F. Chem. Commun. 2003, 1827.
(35) Yi, C. L.; Yang, Y. Q.; Zhu, Y.; Liu, N.; Liu, X. Y.; Lou, J.;Jiang, M. Langmuir 2012, 28 (25), 9218.

[1]	樊晔, 曹崇梅, 方云, 夏咏梅. 自交联共轭亚油酸囊泡基荧光纳米点的构筑及其荧光特性[J]. 物理化学学报, 2022, 38(3): 2002032 - .
[2]	陈灵珊, 洪苑秀, 贺石生, 范震, 杜建忠. 聚(ε-己内酯)-多肽共聚物胶束增强抗生素的抗菌活性[J]. 物理化学学报, 2021, 37(10): 1910059 - .
[3]	王苗, 郑虹宁, 许菲. 异氰酸苯酯诱导的类胶原多肽自组装[J]. 物理化学学报, 2021, 37(10): 1911039 - .
[4]	张静, 王丽娜, 陈晓飞, 王玉峰, 牛成艳, 吴立新, 唐智勇. 氧化还原对Lindqvist型多金属氧簇复合物自组装的动态调控[J]. 物理化学学报, 2020, 36(9): 1912002 - .
[5]	赵亚楠, 何敏, 刘晓芳, 刘斌, 杨建辉. 金二元纳米晶超晶格的自组装和结构表征[J]. 物理化学学报, 2020, 36(9): 1908041 - .
[6]	陈锐杰,李娣,方振远,黄元勇,罗必富,施伟东. In₂O₃三维纳米结构的控制合成及高效光解水产氢活性研究[J]. 物理化学学报, 2020, 36(3): 1903047 - .
[7]	高飞雪, 陈拥军, 刘冬生, 刘鸣华, 田中群, 张希. “可控自组装体系及其功能化”重大研究计划取得系列重要研究成果[J]. 物理化学学报, 2020, 36(11): 2006060 - .
[8]	邢蕊蕊, 邹千里, 闫学海. 肽基超分子胶体[J]. 物理化学学报, 2020, 36(10): 1909048 - .
[9]	肖军燕, 齐利民. 环糊精与表面活性剂主客体作用诱导的金纳米棒可控自组装[J]. 物理化学学报, 2020, 36(10): 1910001 - .
[10]	方佳丽, 陈新, 李唱, 吴玉莲. 原位液体室透射电镜观察金纳米棒/石墨烯复合物的形成和运动过程[J]. 物理化学学报, 2019, 35(8): 808 -815 .
[11]	焦建梅,徐桂英,辛霞. 胆酸盐参与的自组装及微纳米材料制备[J]. 物理化学学报, 2019, 35(7): 684 -696 .
[12]	赵喆, 卢岳, 张振华, 隋曼龄. 原位透射电子显微镜观察电荷驱动的氧化物纳米颗粒水中自组装[J]. 物理化学学报, 2019, 35(5): 539 -545 .
[13]	刘恒昌,冯玉军. CO₂诱导的五嵌段非离子共聚物与阴离子氟碳表面活性剂的相互作用[J]. 物理化学学报, 2019, 35(4): 408 -414 .
[14]	程晓蒙,焦东霞,梁志豪,魏金金,李宏平,杨俊佼. 聚苯乙烯-聚4-乙烯基吡啶两亲嵌段共聚物在CO₂膨胀液体中的组装行为[J]. 物理化学学报, 2018, 34(8): 945 -951 .
[15]	王心怡,谢磊,丁元琪,姚心仪,张弛,孔惠慧,王利坤,许维. 超高真空条件下碱基与金属在Au(111)表面的相互作用[J]. 物理化学学报, 2018, 34(12): 1321 -1333 .