微乳液凝胶及其作为药物载体的研究
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摘要
近年来,随着人们对药物缓释、控释的日益重视,对药物载体的要求也越来越高。微乳液凝胶(microemulsion-based gels,MBGs)以微乳液为基础,兼有微乳液和凝胶的双重优点,可以增强药物的稳定性,提高药物的溶解度和生物利用率,并且由于其粘度较大,对于某些药物,还可以达到缓释,控释的目的,在药剂学领域逐渐受到重视。本论文利用流变学、电镜、荧光等方法,对微乳液凝胶的形成条件、微观结构、流变性质展开研究。此外,研究了Pluronic型嵌段聚合物在bmimBF_4离子液体中的相行为。研究内容主要包括三部分:
第一部分,选择IPM/AOT/Tween85/水形成的W/O微乳液,并向微乳液中加入明胶,形成微乳液凝胶。利用流变和环境扫描电镜研究了明胶和水溶性药物盐酸布替萘芬对微乳液凝胶微观结构的影响。确定了微乳液凝胶形成的最佳条件,即AOT与Tween85的质量比为1:2,并且明胶含量在7.0-12.0 wt%之间。此外,样品的流变参数,如屈服应力值(σ_y)、储能模量(G′)和损耗模量(G″)均随明胶含量的增加而增大,环境扫描电镜也表明当明胶含量在7.0-12.0 wt%之间时,凝胶网络结构较致密。当明胶含量低于7.0 wt%时,体系为溶胶;当明胶含量高于12.0wt%时,明胶过量,会出现胶状和固体状明胶共存的两相。
加入盐酸布替萘芬后,由于AOT和盐酸布替奈芬均与明胶发生静电作用力,这种竞争性静电作用会对微乳液凝胶的网络结构起到一定的破坏作用。但是,盐酸布替萘芬含量为0.5 wt%时,网络结构仍能很好的保持;盐酸布替萘芬含量为1.0 wt%时,会削弱凝胶的网络结构,但是不能完全破坏其网络结构。因此,微乳液凝胶仍然是一种潜在的药物载体。
第二部分,选择IPM/Span20/Tween20/H_2O形成的O/W型微乳液,分别向此微乳液中加入不同链段长度的两亲嵌段聚合物F127(EO_(99)PO_(67)EO_(99))、F68(EO_(70)PO_(30)EO_(79))和L64(EO_(13)PO_(30)EO_(13)),形成温度敏感型微乳液凝胶。对于同一种聚合物来说,形成微乳液凝胶所需的聚合物的量比形成水凝胶所需的聚合物的量少,表明聚合物与表面活性剂之间均存在疏水作用。流变实验中,模量随温度的变化表明,微乳液凝胶的形成与否与微乳液的类型有很大关系,嵌段聚合物在双连续微乳液中并不能形成凝胶,而在水中和O/W的微乳液中均能形成凝胶,这就说明,凝胶的形成必须具备大的连续的水环境,且聚合物在水中和在O/W微乳液中的胶凝机理相似,都是基于嵌段聚合物的胶束化,以及胶束聚集体的形成。
F127与F68形成的微乳液凝胶的解链温度随聚合物含量的增大而升高,L64形成的微乳液凝胶却相反。此外,L64浓度超过48 wt%后,体系在任何温度下均呈流体。荧光实验表明,在F127与F68体系中,芘探针处于微乳液液滴的内核中,证明凝胶形成后,微乳液液滴的结构仍然存在,冷冻蚀刻电镜照片进一步证实,微乳液凝胶体系形成了网络结构,在网络结构中含有大量的微乳液液滴。在L64体系中,芘探针部分处于微乳液的液滴中,部分处于L64的胶束中,微乳液液滴有相当程度的破坏。L64体系之所以与F127和F68体系的相行为有较大差别,是因为L64嵌段聚合物中EO链段很短,EO链段与水分子间形成的氢键较少,氢键作用力较弱.此外,胶束聚集时,EO链段间缠结也会减弱。在L64/微乳液体系中胶束的聚集结构和网络结构比较松散,并且,并不是所有的L64大分子都参与了胶束的形成,在网络结构中存在大量的自由大分子,这些大分子与Span20、Tween20表面活性剂分子间存在相互作用,形成“项链”式结构,穿插于网络结构之中。当L64浓度达到一定程度(＞48 Wt%),L64与水分子呈现一种互溶状态,L64分子基本以单体形式存在,所以在任何温度下均不能形成凝胶。
油溶性药物氯霉素的加入,对F127和F68微乳液凝胶粘弹性的影响不大,微乳液凝胶的网络结构仍能很好的保持,但是对L64微乳液凝胶的网络结构破坏较大。微乳液液滴的存在对于提高油溶性药物的溶解度以及提高体系稳定性方面具有重要的作用。缓释结果表明,微乳液凝胶具有持续释放药物的特性。此外,由于具有温度敏感特性,使得微乳液凝胶比其他药物载体更具有优越性,例如,可以在室温条件下,实现多种给药方式。此外,在本体系中,所选组分均无毒、无刺激性,并且是被药典收录的药用辅料,这种智能型给药体系,在生物医疗方面具有较大的应用潜力。
第三部分,主要考察了离子液体bmimBF_4与嵌段聚合物L64形成的溶致液晶,以及加入不同极性的第三组分对液晶结构的影响。通过双折射性与偏光织构观察以及小角X射线散射等方法,对不同组成、温度条件下形成的有序体系的相态与结构进行表征,并根据分子间的作用力对液晶的形成机理进行了分析。
偏光织构观察和SAXS测试结果表明,在一定浓度和温度下,嵌段聚合物L64可与bmimBF_4离子液体形成层状液晶。bmimBF_4与L64分子间的氢键作用力、静电作用力以及疏溶剂力是液晶形成的驱动力。SAXS结果表明,对于L64/bmimBF_4体系,液晶层间距随L64浓度的增大而减小,这主要是由于表面活性剂浓度的增大,使得溶剂化层中的离子液被挤出所致。
液晶结构受温度影响,温度升高,层间距增大,原因是升温条件下,液晶极性区与非极性区尺寸会有不同程度增大。并且,在一定温度范围内,升温可使液晶区向低聚合物含量方向移动,且体系的有序性增强。但是,随温度的进一步升高,二级散射峰强度变弱,对于所有层状液晶体系,达到某一温度后,偏光性消失,这是因为,温度过高会导致离子液体与PEO链段之间的氢键破坏,从而使结构的有序度降低。
极性不同的分子对层状液晶结构的影响不同。当加入水分子时,水分子插入液晶极性微区,与EO基团氧原子形成氢键,而bmimBF_4与L64形成层状液晶的驱动力是离子液咪唑环阳离子(N~+)与EO基团氧原子上孤对电子间的静电作用力。水分子的加入使得这种静电作用力减弱,从而使得液晶的有序性降低,液晶结构破坏。而加入少量极性较小的油溶性分子后,油溶性分子填充到PPO链段间,使得PPO链段在一定程度上得到伸展,液晶层间距增大,两亲分子排列的有序性增强,这就为油溶性分子的增溶提供了有利条件,扩展了该体系的应用前景。
Recently,the stability and bioavailability of the drug delivery and the controlled drug release have attracted more and more attention.Microemulsion-based gels (MBGs)not only have the characteristics of microemulsion but also the characteristics of gel.MBGs could improve the stability and the bioavailability of the drug and could also control the release of some drugs due to the higher viscosity.In the present study,MBGs are characterized by several techniques including rheological measurements and electron microscope.The formation conditions of MBGs,viscoelastic properties and microstructures of the systems are systematically investigated.Moreover.the phase behaviors of Pluronic copolymer in ionic liquid (bmimBF_4)are investigated.Three main experimental researches are included.
In the first part.gelatin-containing microemulsion-based organogels(MBGs) systems composed of isopropyl myristate(IPM)/AOT/Tween85/H_2O.both with and without a model drug(Butenafine hydrochloride),are investigated by rheological measurements and environmental scanning electron microscope(ESEM).Then the effects of gelatin and butenafine hydrochloride on the rheological properties and microstructures of the MBGs are investigated generally.It is revealed that there exits an optimal gelation concentration of gelatin,homogeneous and compact MBGs can be formed when the concentration of gelatin in the selected W/O microemulsion sample is in the range of 7.0 to 12.0 wt%.Moreover.the rheological properties such as the yield stresses(σ_y).storage and loss moduli(G′.G″)of the samples increase with increasing the concentration of gelatin.Accordingly.the ESEM photographs also reveal that the network structures of MBGs are formed when the concentration of gelatin is between 7.0 and 12.0 wt%.and the network structures become more compact as the concentration of gelatin is increased.At the concentration of gelatin lower than 7.0 wt%,the systems are sols.At the concentration of gelatin higher than 12.0 wt%.the systems are two-phases containing jelly-like phase and solid particles of gelatin.
The addition of butenafine hydrochloride to the MBGs could weaken the interconnected network structures of the system at a certain extent.Namely,when the concentration of butenafine hydrochloride is lower than 0.5 wt%,the network structures of MBGs could be maintained perfectly.Consequently,the systems are potentially transdermal drug delivery vehicles.At the higher butenafine hydrochloride concentration(1.0 wt%),the effect of butenafine hydrochloride on the weaken network structures of MBGs is obvious,but the networks have not been destroyed completely.
In the second part,temperature-sensitive microemulsion-based gels(MBGs)of three copolymers of different composition,F127(EO_(99)PO_(67)EO_(99)),F68(EO_(79)PO_(30)EO_(79)) and L64(EO_(13)PO_(30)EO_(13)),are formed in microemulsion systems composed of isopropyl myristate(IPM)/Span20/Tween20/H_2O,and the phase behaviors of the systems are investigated.For the same polymer,the gelation concentration of copolymer is much lower in MBGs than in hydrogels which indicates that there are hydrophobic interactions between copolymer and surfactant molecules,so the micelles easily pack and turn into gels.Temperature sweep measurements indicate that the type of microemulsion is important for the formation of MBG.The gelation can not form in B.C.microemulsion,but can form in O/W microemulsion and water. this suggests that the enough amount water is very important for forming copolymer micelles and the micelles are formed in the water phase of the O/W microemulsion. The gelation mechanism of MBGs is similar to that of hydrogels,both based on the micellization and aggregation of micelles.
The melting temperatures of MBGs increase with increasing F127 or F68 concentration,while the MBGs formed by L64 are opposite.Moreover,when the concentration of L64 is more than 48 wt%,the systems are liquid at any temperature. In F127 and F68 systems,the results of fluorescent experiments suggest that pyrene is located in the core of the microemulsion droplet,and the major structure of the microemulsion is retained after formation MBGs,which is further proved by FF-TEM photographs.In L64 systems,some pyrene is located in the core of the microemulsion droplet,some is located in micelles of L64.and the structure of the microemulsion is destroyed at a considerable extent.There are very different phase behaviors between L64 with F127 or F68 systems,which is because that the hydrogen bonds between EO and H_2O are much less due to the shorter EO chains of L64,so hydrogen bonds force is weak.Moreover,the entanglement of EO chains is weakened due to the shorter EO chains.Therefore,the network structure is much looser.Furthermore,there are many free L64 macromolecules in the network structure,so there are some necklace-like structures formed by L64 macromolecules and the surfactants(Span20.Tween20). When the concentration of L64 reaches a certain level(＞48 wt%),L64 macromolecules and water molecules are miscible,and L64 exists as monomer.so the MBGs are not formed at any temperature.
Chloramphenicol has little effect on the rheological properties of the MBGs formed by F127 and F68,and the network structures of MBGs are still retained. While the network structures of MBGs formed by L64 are destroyed at a certain extent after the addition of chloramphenicol into the systems.The continued existence of microemulsion droplets plays an important role in enhancing the solubility and stability of oil-soluble drugs.The results of controlled release experiments suggest that MBG shows sustained release properties.Moreover.due to its temperature-sensitivity.MBG is superior to other drug carriers,e.g.multiple administrations are much easier to achieve at room temperature.Furthermore.in these systems,the formulations have low toxicity and are approved for pharmaceutical use. so the MBG systems have potential as drug delivery systems.
In the last part,lyotropic liquid crystalline(LLC)made of nonionic block copolymer L64 and ionic liquid(ILs)bmimBF_4(1-n-butyl-3-methyl imidazolium tetrafluoroborate)is constructed and characterized by POM and SAXS measurements. with comparison of component and temperature effects.Moreover.the formation mechanism is discussed.
POM and SAXS measurements indicate that lamellar phase can be obtained with increasing L64 concentration at a certain temperature range.The various interactions between PEO-bmimBF_4(hydrogen bonding)and PPO-bmimBF_4(hydrophobic interaction)play the key role in LLC formation.The results of SAXS suggest that the lattice spacing(d)decrease with increasing L64 concentration.
The effect of temperature on the lamellar phase is investigated.The lattice spacing increases with increasing temperature.This change can be attributed to swelling of polar and apolar microdomains.At certain temperature range,the lamellar region shifts to lower polymer concentrations and the lamellar phase becomes more ordered with increasing temperature.However,the birefringent phenomenon of the lamellar phase disappears when the temperature reaches a certain level,which is attributed to the breakage of hydrogen bonds between bmimBF_4 and EO chains.So the long-range order of LLC is decreased.
The effect of different polarity molecules on the lamellar phase is also investigated.With addition water,water molecules insert into the polar microdomains of LLC,and form hydrogen bonds with the oxygen atom of EO groups.The static actions which occur between the cation moiety(-N~+)of IL and the lone pairs on oxygen atom of EO groups are the key driving force for the formation of LLC.The addition of water molecules makes the static actions weaken and the long-range order of LLC decrease.However,after addition a little apolar molecules,apolar molecules insert into hydrophobic microdomains(PPO chains),which makes PPO chains extend at certain degree,and the order of LLC increases.Therefore,the systems will supply favorable conditions for enhancing the solubility of oil-soluble molecules,which further expands application prospects of the systems.
第一部分,选择IPM/AOT/Tween85/水形成的W/O微乳液,并向微乳液中加入明胶,形成微乳液凝胶。利用流变和环境扫描电镜研究了明胶和水溶性药物盐酸布替萘芬对微乳液凝胶微观结构的影响。确定了微乳液凝胶形成的最佳条件,即AOT与Tween85的质量比为1:2,并且明胶含量在7.0-12.0 wt%之间。此外,样品的流变参数,如屈服应力值(σ_y)、储能模量(G′)和损耗模量(G″)均随明胶含量的增加而增大,环境扫描电镜也表明当明胶含量在7.0-12.0 wt%之间时,凝胶网络结构较致密。当明胶含量低于7.0 wt%时,体系为溶胶;当明胶含量高于12.0wt%时,明胶过量,会出现胶状和固体状明胶共存的两相。
加入盐酸布替萘芬后,由于AOT和盐酸布替奈芬均与明胶发生静电作用力,这种竞争性静电作用会对微乳液凝胶的网络结构起到一定的破坏作用。但是,盐酸布替萘芬含量为0.5 wt%时,网络结构仍能很好的保持;盐酸布替萘芬含量为1.0 wt%时,会削弱凝胶的网络结构,但是不能完全破坏其网络结构。因此,微乳液凝胶仍然是一种潜在的药物载体。
第二部分,选择IPM/Span20/Tween20/H_2O形成的O/W型微乳液,分别向此微乳液中加入不同链段长度的两亲嵌段聚合物F127(EO_(99)PO_(67)EO_(99))、F68(EO_(70)PO_(30)EO_(79))和L64(EO_(13)PO_(30)EO_(13)),形成温度敏感型微乳液凝胶。对于同一种聚合物来说,形成微乳液凝胶所需的聚合物的量比形成水凝胶所需的聚合物的量少,表明聚合物与表面活性剂之间均存在疏水作用。流变实验中,模量随温度的变化表明,微乳液凝胶的形成与否与微乳液的类型有很大关系,嵌段聚合物在双连续微乳液中并不能形成凝胶,而在水中和O/W的微乳液中均能形成凝胶,这就说明,凝胶的形成必须具备大的连续的水环境,且聚合物在水中和在O/W微乳液中的胶凝机理相似,都是基于嵌段聚合物的胶束化,以及胶束聚集体的形成。
F127与F68形成的微乳液凝胶的解链温度随聚合物含量的增大而升高,L64形成的微乳液凝胶却相反。此外,L64浓度超过48 wt%后,体系在任何温度下均呈流体。荧光实验表明,在F127与F68体系中,芘探针处于微乳液液滴的内核中,证明凝胶形成后,微乳液液滴的结构仍然存在,冷冻蚀刻电镜照片进一步证实,微乳液凝胶体系形成了网络结构,在网络结构中含有大量的微乳液液滴。在L64体系中,芘探针部分处于微乳液的液滴中,部分处于L64的胶束中,微乳液液滴有相当程度的破坏。L64体系之所以与F127和F68体系的相行为有较大差别,是因为L64嵌段聚合物中EO链段很短,EO链段与水分子间形成的氢键较少,氢键作用力较弱.此外,胶束聚集时,EO链段间缠结也会减弱。在L64/微乳液体系中胶束的聚集结构和网络结构比较松散,并且,并不是所有的L64大分子都参与了胶束的形成,在网络结构中存在大量的自由大分子,这些大分子与Span20、Tween20表面活性剂分子间存在相互作用,形成“项链”式结构,穿插于网络结构之中。当L64浓度达到一定程度(＞48 Wt%),L64与水分子呈现一种互溶状态,L64分子基本以单体形式存在,所以在任何温度下均不能形成凝胶。
油溶性药物氯霉素的加入,对F127和F68微乳液凝胶粘弹性的影响不大,微乳液凝胶的网络结构仍能很好的保持,但是对L64微乳液凝胶的网络结构破坏较大。微乳液液滴的存在对于提高油溶性药物的溶解度以及提高体系稳定性方面具有重要的作用。缓释结果表明,微乳液凝胶具有持续释放药物的特性。此外,由于具有温度敏感特性,使得微乳液凝胶比其他药物载体更具有优越性,例如,可以在室温条件下,实现多种给药方式。此外,在本体系中,所选组分均无毒、无刺激性,并且是被药典收录的药用辅料,这种智能型给药体系,在生物医疗方面具有较大的应用潜力。
第三部分,主要考察了离子液体bmimBF_4与嵌段聚合物L64形成的溶致液晶,以及加入不同极性的第三组分对液晶结构的影响。通过双折射性与偏光织构观察以及小角X射线散射等方法,对不同组成、温度条件下形成的有序体系的相态与结构进行表征,并根据分子间的作用力对液晶的形成机理进行了分析。
偏光织构观察和SAXS测试结果表明,在一定浓度和温度下,嵌段聚合物L64可与bmimBF_4离子液体形成层状液晶。bmimBF_4与L64分子间的氢键作用力、静电作用力以及疏溶剂力是液晶形成的驱动力。SAXS结果表明,对于L64/bmimBF_4体系,液晶层间距随L64浓度的增大而减小,这主要是由于表面活性剂浓度的增大,使得溶剂化层中的离子液被挤出所致。
液晶结构受温度影响,温度升高,层间距增大,原因是升温条件下,液晶极性区与非极性区尺寸会有不同程度增大。并且,在一定温度范围内,升温可使液晶区向低聚合物含量方向移动,且体系的有序性增强。但是,随温度的进一步升高,二级散射峰强度变弱,对于所有层状液晶体系,达到某一温度后,偏光性消失,这是因为,温度过高会导致离子液体与PEO链段之间的氢键破坏,从而使结构的有序度降低。
极性不同的分子对层状液晶结构的影响不同。当加入水分子时,水分子插入液晶极性微区,与EO基团氧原子形成氢键,而bmimBF_4与L64形成层状液晶的驱动力是离子液咪唑环阳离子(N~+)与EO基团氧原子上孤对电子间的静电作用力。水分子的加入使得这种静电作用力减弱,从而使得液晶的有序性降低,液晶结构破坏。而加入少量极性较小的油溶性分子后,油溶性分子填充到PPO链段间,使得PPO链段在一定程度上得到伸展,液晶层间距增大,两亲分子排列的有序性增强,这就为油溶性分子的增溶提供了有利条件,扩展了该体系的应用前景。
Recently,the stability and bioavailability of the drug delivery and the controlled drug release have attracted more and more attention.Microemulsion-based gels (MBGs)not only have the characteristics of microemulsion but also the characteristics of gel.MBGs could improve the stability and the bioavailability of the drug and could also control the release of some drugs due to the higher viscosity.In the present study,MBGs are characterized by several techniques including rheological measurements and electron microscope.The formation conditions of MBGs,viscoelastic properties and microstructures of the systems are systematically investigated.Moreover.the phase behaviors of Pluronic copolymer in ionic liquid (bmimBF_4)are investigated.Three main experimental researches are included.
In the first part.gelatin-containing microemulsion-based organogels(MBGs) systems composed of isopropyl myristate(IPM)/AOT/Tween85/H_2O.both with and without a model drug(Butenafine hydrochloride),are investigated by rheological measurements and environmental scanning electron microscope(ESEM).Then the effects of gelatin and butenafine hydrochloride on the rheological properties and microstructures of the MBGs are investigated generally.It is revealed that there exits an optimal gelation concentration of gelatin,homogeneous and compact MBGs can be formed when the concentration of gelatin in the selected W/O microemulsion sample is in the range of 7.0 to 12.0 wt%.Moreover.the rheological properties such as the yield stresses(σ_y).storage and loss moduli(G′.G″)of the samples increase with increasing the concentration of gelatin.Accordingly.the ESEM photographs also reveal that the network structures of MBGs are formed when the concentration of gelatin is between 7.0 and 12.0 wt%.and the network structures become more compact as the concentration of gelatin is increased.At the concentration of gelatin lower than 7.0 wt%,the systems are sols.At the concentration of gelatin higher than 12.0 wt%.the systems are two-phases containing jelly-like phase and solid particles of gelatin.
The addition of butenafine hydrochloride to the MBGs could weaken the interconnected network structures of the system at a certain extent.Namely,when the concentration of butenafine hydrochloride is lower than 0.5 wt%,the network structures of MBGs could be maintained perfectly.Consequently,the systems are potentially transdermal drug delivery vehicles.At the higher butenafine hydrochloride concentration(1.0 wt%),the effect of butenafine hydrochloride on the weaken network structures of MBGs is obvious,but the networks have not been destroyed completely.
In the second part,temperature-sensitive microemulsion-based gels(MBGs)of three copolymers of different composition,F127(EO_(99)PO_(67)EO_(99)),F68(EO_(79)PO_(30)EO_(79)) and L64(EO_(13)PO_(30)EO_(13)),are formed in microemulsion systems composed of isopropyl myristate(IPM)/Span20/Tween20/H_2O,and the phase behaviors of the systems are investigated.For the same polymer,the gelation concentration of copolymer is much lower in MBGs than in hydrogels which indicates that there are hydrophobic interactions between copolymer and surfactant molecules,so the micelles easily pack and turn into gels.Temperature sweep measurements indicate that the type of microemulsion is important for the formation of MBG.The gelation can not form in B.C.microemulsion,but can form in O/W microemulsion and water. this suggests that the enough amount water is very important for forming copolymer micelles and the micelles are formed in the water phase of the O/W microemulsion. The gelation mechanism of MBGs is similar to that of hydrogels,both based on the micellization and aggregation of micelles.
The melting temperatures of MBGs increase with increasing F127 or F68 concentration,while the MBGs formed by L64 are opposite.Moreover,when the concentration of L64 is more than 48 wt%,the systems are liquid at any temperature. In F127 and F68 systems,the results of fluorescent experiments suggest that pyrene is located in the core of the microemulsion droplet,and the major structure of the microemulsion is retained after formation MBGs,which is further proved by FF-TEM photographs.In L64 systems,some pyrene is located in the core of the microemulsion droplet,some is located in micelles of L64.and the structure of the microemulsion is destroyed at a considerable extent.There are very different phase behaviors between L64 with F127 or F68 systems,which is because that the hydrogen bonds between EO and H_2O are much less due to the shorter EO chains of L64,so hydrogen bonds force is weak.Moreover,the entanglement of EO chains is weakened due to the shorter EO chains.Therefore,the network structure is much looser.Furthermore,there are many free L64 macromolecules in the network structure,so there are some necklace-like structures formed by L64 macromolecules and the surfactants(Span20.Tween20). When the concentration of L64 reaches a certain level(＞48 wt%),L64 macromolecules and water molecules are miscible,and L64 exists as monomer.so the MBGs are not formed at any temperature.
Chloramphenicol has little effect on the rheological properties of the MBGs formed by F127 and F68,and the network structures of MBGs are still retained. While the network structures of MBGs formed by L64 are destroyed at a certain extent after the addition of chloramphenicol into the systems.The continued existence of microemulsion droplets plays an important role in enhancing the solubility and stability of oil-soluble drugs.The results of controlled release experiments suggest that MBG shows sustained release properties.Moreover.due to its temperature-sensitivity.MBG is superior to other drug carriers,e.g.multiple administrations are much easier to achieve at room temperature.Furthermore.in these systems,the formulations have low toxicity and are approved for pharmaceutical use. so the MBG systems have potential as drug delivery systems.
In the last part,lyotropic liquid crystalline(LLC)made of nonionic block copolymer L64 and ionic liquid(ILs)bmimBF_4(1-n-butyl-3-methyl imidazolium tetrafluoroborate)is constructed and characterized by POM and SAXS measurements. with comparison of component and temperature effects.Moreover.the formation mechanism is discussed.
POM and SAXS measurements indicate that lamellar phase can be obtained with increasing L64 concentration at a certain temperature range.The various interactions between PEO-bmimBF_4(hydrogen bonding)and PPO-bmimBF_4(hydrophobic interaction)play the key role in LLC formation.The results of SAXS suggest that the lattice spacing(d)decrease with increasing L64 concentration.
The effect of temperature on the lamellar phase is investigated.The lattice spacing increases with increasing temperature.This change can be attributed to swelling of polar and apolar microdomains.At certain temperature range,the lamellar region shifts to lower polymer concentrations and the lamellar phase becomes more ordered with increasing temperature.However,the birefringent phenomenon of the lamellar phase disappears when the temperature reaches a certain level,which is attributed to the breakage of hydrogen bonds between bmimBF_4 and EO chains.So the long-range order of LLC is decreased.
The effect of different polarity molecules on the lamellar phase is also investigated.With addition water,water molecules insert into the polar microdomains of LLC,and form hydrogen bonds with the oxygen atom of EO groups.The static actions which occur between the cation moiety(-N~+)of IL and the lone pairs on oxygen atom of EO groups are the key driving force for the formation of LLC.The addition of water molecules makes the static actions weaken and the long-range order of LLC decrease.However,after addition a little apolar molecules,apolar molecules insert into hydrophobic microdomains(PPO chains),which makes PPO chains extend at certain degree,and the order of LLC increases.Therefore,the systems will supply favorable conditions for enhancing the solubility of oil-soluble molecules,which further expands application prospects of the systems.
引文
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