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纸质出版日期:2008-11-20,
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赵长稳, 庄秀丽, 陈学思, 景遐斌. 温度敏感性PNIPAM-b-PZLL-b-mPEG三嵌段共聚物的合成与自组装研究[J]. 高分子学报, 2008,(11):1096-1101.
ZHAO Changwen, ZHUANG Xiuli, CHEN Xuesi, JING Xiabin. SYNTHESIS AND SELF-ASSEMBLY OF POLY(N-ISOPROPYLACRYLAMIDE)-b-POLY(ε-BENZYLOXYCARBONYL-L-LYSINE)-b-POLY(ETHYLENE GLYCOL)[J]. Acta Polymerica Sinica, 2008,(11):1096-1101.
赵长稳, 庄秀丽, 陈学思, 景遐斌. 温度敏感性PNIPAM-b-PZLL-b-mPEG三嵌段共聚物的合成与自组装研究[J]. 高分子学报, 2008,(11):1096-1101. DOI: 10.3724/SP.J.1105.2008.01096.
ZHAO Changwen, ZHUANG Xiuli, CHEN Xuesi, JING Xiabin. SYNTHESIS AND SELF-ASSEMBLY OF POLY(N-ISOPROPYLACRYLAMIDE)-b-POLY(ε-BENZYLOXYCARBONYL-L-LYSINE)-b-POLY(ETHYLENE GLYCOL)[J]. Acta Polymerica Sinica, 2008,(11):1096-1101. DOI: 10.3724/SP.J.1105.2008.01096.
通过大分子引发剂引发ε-苄氧羰基-L-赖氨酸-N-羧酸酐(Lys-NCA)开环聚合和大分子缩合的方法合成了聚(N-异丙基丙烯酰胺)-b-聚(ε-苄氧羰基-L-赖氨酸)-b-聚乙二醇单甲醚三嵌段共聚物(PNIPAM-b-PZLL-b-mPEG).用GPC和1H-NMR对其结构进行了表征.用芘荧光探针法证明了该三嵌段聚合物形成胶束的性质并测定了临界胶束浓度(CMC).动态光散射(DLS)研究表明,在固定PNIPAM-b-PZLL链段长度的情况下,mPEG分子量为2000时,胶束在温度高于临界溶解温度(LCST)时发生聚集,mPEG分子量为5000时,胶束在LCST以上没有发生聚集.
A novel amphiphilic and thermosensitive triblock copolymer of poly(N-isopropylacrylamide)-b-poly(3-benzyloxycarbonyl-L-lysine)-b-poly(ethylene glycol) (PNIPAM-b-PZLL-b-mPEG) with designed molecular weight and narrow molecular weight distribution was prepared.Synthetic procedure included the following steps.(1) Amino-terminated PNIPAM was synthesized via the free radical polymerization of NIPAM in methanol using 2
2′-azobisisobutyronitrile (AIBN) and 2-aminoethanethiol hydrochloride (AET#8226;HCl) as the initiator and chain transfer agent
respectively.Its molecular weight was calculated by the 1H-NMR-spectra in D2O.(2) The block copolymers
PNIPAM-b-PZLL were synthesized by the ringopening polymerization (ROP) of 3-benzyloxycarbonyl-L-lysine N-carboxyanhydride (Z-Lys-NCA) with PNIPAMNH2 as a macroinitiator.Their structure was confirmed by the 1H-NMR spectra.The molecular weight and molecular weight distribution of PNIPAM-b-PZLL were characterized by GPC analysis in THF.The relatively narrow polydispersity of the obtained PNIPAM-b-PZLL could be explained by the living character of the ROP of NCAs initiated by primary amine hydrochlorides which avoided the side reaction called “active monomer" mechanism.Generally
the molecular weights could be controlled by the feed molar ratios of monomer to maroinitiator.(3) For preparing the triblock polymers
PNIPAM-b-PZLL-b-mPEG
it was necessary to convert the terminal hydroxyl group of mPEG of different molecular weight (2000 or 5000) into carboxyl group by succinic anhydride.Its 1H-NMR spectra showed this was a high efficiency reaction.Then the triblock copolymers were obtained by the condensation reaction between carboxyl-capped mPEG and aminocapped PNIPAM-b-PZLL in the presence of dicyclohexylcarbodiimide (DCC) and 4-dimethylaminopyridine (DMAP).The 1H-NMR confirmed their structure.Based on the integration ratio
their relative amount in the copolymer was calculated.And their Mn(NMR) agreed well with the theoretical numberaverage molecular weight.GPC analysis in THF revealed a monomodal and symmetric peak which showed the successful synthesis of target copolymers.All the molecular weight distributions (Mw/Mn=1.11~1.20) were relatively narrow.The triblock copolymer could selfassemble into micelles in aqueous solution with hydrophobic PZLL as the core- and hydrophilic PNIPAM and mPEG as the corona.Its critical micelle concentration (CMC) was measured by a fluorescence spectra technique using pyrene as a probe.The CMC decreased with the increase of PZLL content and increased with the increase of PEG content.Dynamic light scattering (DLS) analyses of triblock copolymer micelles revealed their size of less than 100 nm and narrow size distribution.It is well-known that PNIPAM homopolymer dissolved in cold and dilute aqueous solution but gets insoluble at ca. 32℃ due to its lower critical solution temperature (LCST) phase behavior.When the temperature was above the LCST
the PNIPAM undergoes a reversible phase transition caused by the coil-to-globule transition and becomes more hydrophobic.So changing temperature will influence the stability of micelles.As anticipated
the micelles aggregated at temperatures above LCST when the Mn of mPEG was 2000.That is probably that the mPEG2000 could not prevent the intermicellar hydrophobic interaction.However
no obvious aggregation of micelles was found at temperatures above LCST when the Mn of mPEG was 5000 because the hydrophobic interaction between the micelles was prevented by mPEG5000 effectively.
聚(N-异丙基丙烯酰胺)聚(ε-苄氧羰基-L-赖氨酸)聚乙二醇单甲醚温度敏感性胶束
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