分散液滴的尺寸对含水和非水微乳体系临界行为的影响
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摘要
本文采用“折射率法”测定了具有不同液滴尺寸的含水微乳体系(水／AOT／正癸烷)和非水微乳体系(DMA／AOT／正辛烷)的温度-折射率(T，n)共存曲线，根据标准曲线将其转化为温度-体积分数(T，φ)和温度-有效体积分数(T，ψ)共存曲线，并由共存曲线推导出临界指数β，指前因子B，Wegner校正项B_1及共存曲线直径ρ_d。分别研究含水微乳体系和非水微乳体系的临界行为，并讨论了分散液滴的尺寸对两类体系临界行为的影响，主要结论如下：
(1)水／AOT／正癸烷体系具有低临界温度，且临界温度随分散液滴尺寸的增加而降低；而DMA／AOT／正辛烷体系具有高临界温度，临界温度均随分散液滴尺寸的增加而增大。前者相变主要是受焓变控制，而后者是受熵变控制。
(2)水／AOT／正癸烷体系和DMA／AOT／正辛烷体系的临界组成均随着液滴尺寸的增加而略有降低。
(3)水／AOT／正癸烷各体系的临界指数β在温度接近临界温度时，均趋近于3D-Ising模型的理论值0.3265；而DMA／AOT／正辛烷各体系在本论文所研究的ω_s范围内，临界指数β在较宽的温度范围内均接近于Fisher重整化理论值0.365。两者不同可能的原因在于后者ω较大时，极少量DMA溶解在正辛烷中，导致临界指数β重正化。两者的共同点是分散液滴尺寸的改变均不影响体系的临界指数值。
(4)水／AOT／正癸烷体系和DMA／AOT／正辛烷微乳体系的指前因子B均随分散液滴尺寸的增加而增大，这可能归因于液滴间相互作用的增加导致临界指数B增大。
The coexistence curves (T, n) (T, n are temperature and refractive index, respectively) of water/l,4-di(2-ethyl-l-hexyl)sulphosuccinate(AOT)/decane and dimethylacetamide (DMA)/AOT/octane with different droplet sizes were determined by measurements of refractive indexes of coexisting phases at constant pressure for various temperatures in the critical regions. The coexistence curves of (T, n) were converted to the coexistence curves of (T,φ) and (T,Ψ), (φandΨare volume fraction and effective volume fraction, respectively) by the standard curves. The critical exponentsβ, the critical amplitudes B, the amplitude of Wegner correction terms B_1 and the diameters of coexistence curvesρ_d were deduced from the coexistence curves. The effects of the dispersed droplet sizes on the critical behavior of aqueous and nonaqueous microemulsions were discussed. The experimental results are summarized as follows:
(1) All the aqueous microemulsions (AM) have the lower critical temperatures which decrease as the disperse droplet sizes increase; on the contrary, the upper critical temperatures increases with the dispersed droplet sizes for all the nonaqueous microemulsions (NM). The phase transition for the former is controlled by the change of enthalpy, but the latter is controlled by the change of entropy.
(2) The critical volume fractions little decrease with the increase of the dispersed droplet sizes for the AM systems and NM systems.
(3) The values ofβapproach the 3D-Ising value of 0.3265 for all the AM systems in the regions sufficiently close to the critical temperatures and the Fisher's Renormalization value of 0.365 for all the NM systems. Two types of systems belong to the different universal classes that may be attributed to the solubilization of DMA in the octane, which induces the critical exponentβto be renormalized. The values of critical exponebtsβfor both AM and NM are not affected by the change of the dispersed droplet sizes.
(4) The system-dependence amplitudes B of both AM and NM almost linearly increase with the dispersed droplet sizes which are ascribed to the increase of interaction between the droplets.
(1)水／AOT／正癸烷体系具有低临界温度，且临界温度随分散液滴尺寸的增加而降低；而DMA／AOT／正辛烷体系具有高临界温度，临界温度均随分散液滴尺寸的增加而增大。前者相变主要是受焓变控制，而后者是受熵变控制。
(2)水／AOT／正癸烷体系和DMA／AOT／正辛烷体系的临界组成均随着液滴尺寸的增加而略有降低。
(3)水／AOT／正癸烷各体系的临界指数β在温度接近临界温度时，均趋近于3D-Ising模型的理论值0.3265；而DMA／AOT／正辛烷各体系在本论文所研究的ω_s范围内，临界指数β在较宽的温度范围内均接近于Fisher重整化理论值0.365。两者不同可能的原因在于后者ω较大时，极少量DMA溶解在正辛烷中，导致临界指数β重正化。两者的共同点是分散液滴尺寸的改变均不影响体系的临界指数值。
(4)水／AOT／正癸烷体系和DMA／AOT／正辛烷微乳体系的指前因子B均随分散液滴尺寸的增加而增大，这可能归因于液滴间相互作用的增加导致临界指数B增大。
The coexistence curves (T, n) (T, n are temperature and refractive index, respectively) of water/l,4-di(2-ethyl-l-hexyl)sulphosuccinate(AOT)/decane and dimethylacetamide (DMA)/AOT/octane with different droplet sizes were determined by measurements of refractive indexes of coexisting phases at constant pressure for various temperatures in the critical regions. The coexistence curves of (T, n) were converted to the coexistence curves of (T,φ) and (T,Ψ), (φandΨare volume fraction and effective volume fraction, respectively) by the standard curves. The critical exponentsβ, the critical amplitudes B, the amplitude of Wegner correction terms B_1 and the diameters of coexistence curvesρ_d were deduced from the coexistence curves. The effects of the dispersed droplet sizes on the critical behavior of aqueous and nonaqueous microemulsions were discussed. The experimental results are summarized as follows:
(1) All the aqueous microemulsions (AM) have the lower critical temperatures which decrease as the disperse droplet sizes increase; on the contrary, the upper critical temperatures increases with the dispersed droplet sizes for all the nonaqueous microemulsions (NM). The phase transition for the former is controlled by the change of enthalpy, but the latter is controlled by the change of entropy.
(2) The critical volume fractions little decrease with the increase of the dispersed droplet sizes for the AM systems and NM systems.
(3) The values ofβapproach the 3D-Ising value of 0.3265 for all the AM systems in the regions sufficiently close to the critical temperatures and the Fisher's Renormalization value of 0.365 for all the NM systems. Two types of systems belong to the different universal classes that may be attributed to the solubilization of DMA in the octane, which induces the critical exponentβto be renormalized. The values of critical exponebtsβfor both AM and NM are not affected by the change of the dispersed droplet sizes.
(4) The system-dependence amplitudes B of both AM and NM almost linearly increase with the dispersed droplet sizes which are ascribed to the increase of interaction between the droplets.
引文
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