摘要
一般而言,常用聚合物材料不仅需要将几种大分子流体混合在一起,而且需要加入固体“填料”粒子。这些多组分聚合物体系的形态结构决定其使用性能,而多组分聚合物体系的相行为在很大程度上决定了其形态结构的形成和演化。因此,对多组分聚合物体系相行为的研究无疑具有重大的学术价值和应用价值。常规的研究方法,如差示扫描量热法(DSC)、动态力学分析法(DMA)、荧光光谱法、傅立叶转换红外光谱法(FTIR)、小角X射线散射(SAXS)、小角中子散射(SANS)和小角激光散射(SALS)等,都存在不可避免的缺陷。为了克服这些研究方法的缺陷,本论文采用了一种较为新颖的方法—动态流变学方法。其理论依据在于:多组分聚合物体系的流变行为与组分间的相互作用、相形态结构密切相关,流变响应能够准确地反映相形态结构的形成和演化。为此,本论文首先用动态流变学方法研究了PMMA/SAN二元聚合物共混体系的相行为,然后将其推广到PMMA/SAN/SiO_2三元共混体系,成功地探索出了一条研究多组分聚合物体系特别是含填料的三元共混体系相行为的新途径。本论文的主要工作和结论如下:
1.选择PMMA/SAN二元体系,系统地探讨了该体系的线性动态粘弹响应与其特定的相行为之间的关系,结果表明:(1)二元聚合物共混体系在均相区符合时-温叠加原理;而在过渡区开始出现热流变复杂性,表现为时-温叠加原理失效、弹性显著增加和松弛时间明显增长,而且储能模量G′的热流变复杂性比损耗模量G″更加显著。(2)利用动态温度扫描测试能够一次性获得二元聚合物共混体系的Binodal和Spinodal相分离温度。(3)PMMA/SAN共混体系的临
四川大学博士论文
界组成为56/44,临界温度为184.0℃;热力学相互作用参数x,的温度依赖行为
可以表示为z。(T)二0.017一6.442/T,由此外推出体系在室温下的x吞为一。.0046,
与其他研究者用SANS法确定的X全一0.01比较接近。
2.通过将成核和生长相分离过程引入到简化Palicmc乳液模型中研究了
PMM刀sAN(80/20)体系的成核和生长相分离动力学,并探讨了在临界组成共混
体系PMMA/s AN(56/44)中线性动态流变测试对其SPinodal相分离过程的影响,
结果表明:(l)二元聚合物共混体系在进行成核和生长相分离时也存在类似
SPinodal相分离中出现的相分离延迟时间。(2)在系列低频动态时间扫描
(G’一Tim。)曲线中,随着频率的增加,口的时间依赖行为逐渐变得不明显;
而且在相分离初期,G’随时间迅速增加,而后增加的幅度渐缓。(3)即使是线
性振荡剪切也会影响共连续相形态结构的发展,动态流变学方法不适于研究聚
合物共混体系在spinodal相分离中微区的粗化行为。(4)pMMA/SAN(80/20)
体系分散相微区的生长指数为0.366,稍大于Lifshitz一Slyozov机理的1/3。
3.选择PMM刀SAN/5102一5体系,首次用动态流变学方法确定了含填料的
三元共混体系的相界,结果发现:(l)与二元聚合物共混体系类似,含填料的
三元共混体系在过渡区开始出现热流变复杂性,表现为时一温叠加原理失效、弹
性显著增加和松弛时间明显增长,而且储能模量口的热流变复杂性比损耗模量
G”的更加显著。(2) 510:活性填料的引入使得PMM刀SAN基体的相分离温度
提高了;在PMM刀SAN/Si仇一5体系中,PMMA与SAN链段间的热力学相互作
用参数x。与温度之间的关系为x,(T)二0.014一5.031/T,由此得到室温下的石
为一0 .0026。
4.首次以vignaux一Nassiet和Palierne两个乳液模型为基础推导出聚合物/
聚合物/填料三元共混体系的乳液模型,通过相分离过程的引入初步探讨了
PMM刀sAN(80220)25102一5和PMM刀sAN(20/50)25102一5两个体系的成核和生长
相分离动力学,结果表明:与二元聚合物共混体系相比,引入活性填料粒子后
的三元共混体系的相分离延迟时间和相分离动力学都取决于活性填料粒子是选
择性吸附连续相聚合物还是分散相聚合物。当活性填料粒子选择性吸附连续相
聚合物时,相分离延迟时间有所缩短:而且相分离速度有所加快,如
PMMA/sAN(80/2 0)/5102一5体系分散相微区的生长指数为0.379。当活性填料粒
子选择性吸附分散相聚合物时,相分离延迟时间大大缩短,而且相分离出现快
二元聚合物及含填料的三元共混体系相行为的动态流变学研究
生长和微区尺寸饱和两个阶段:在快生长阶段,复合分散相微区的生长指数远
大于l/3,相分离速度大大加快,如PMMA/SAN(20/80)/5102一5体系分散相微区
的生长指数为0.649;而在饱和阶段,复合分散相微区的粗化被抑制。
5.首次在Flory一Huggins平均场理论的基础上系统地推导出聚合物/聚合物
/填料体系的热力学方程,并且模拟了活性填料对二元聚合物共混体系热力学稳
定性的影响,结果表明:(1)活性填料的引入可能使二元聚合物共混体系的热
力学稳定性提高,也可能降低。这取决于聚合物共混体系本身的热力学稳定性、
聚合物组分与填料表面功能基团之间的相互作用强度和共混组成。(2)当活性
填料的含量低于某一临界值时,表面层和基体共存,活性填料的引入使不相容
聚合物共混体系的热力学稳定性提高,而且活性填料含量越多越明显;如果?
The commonly used polymer materials are usually manufactured not only by mixing several macromolecular fluids, but also by incorporating solid "filler" particles. The final properties of the multicomponent polymer systems depend on their final morphology and structure whose formation and development is largely dependent on their phase behavior on the investigation of which, therefore, a great value is placed from the academic and commercial viewpoint. The common research techniques used in this area, such as differential scan calorimetry (DSC), dynamic mechanical analysis (DMA), fluorescence spectrum, Fourier-transform infrared ray (FTIR), small angle X-ray scattering (SAXS), small angle neutron scattering (SANS) and small angle laser sacattering (SALS) and so forth, have intrinsic drawbacks. To eliminate the drawbacks from those techniques, here a comparatively new technique based on dynamic rheology, was adopted, which is theoretically on the basis of the fact that the dynamic rheological behavior of multicomponent polymer systems is countless tied to both the interactions between the blending components and their phase morphology and structure, and in return their dynamic rheological behavior is able to precisely probe the formation and evolution of their phase morphology and structure. Thus, the phase behavior of PMMA/SAN blends was first investigated by dynamic rheological measurements; such investigations were then extended to PMMA/SAN/SiO_(2) systems to explore the influence of active fillers on the phase behavior of binary polymer blends. Hereafter, an innovative way to examine the phase behavior of the multicomponent polymer blends, especially the ternary mixtures containing fillers, has successfully been sought out in this thesis. The main work and conclusions are as follows.
1. The relationship between the linear dynamic viscoelastic response of PMMA/SAN blends and their corresponding phase behavior were systematically explored in Chapter 3. The following statements can be made: (1) In the homogeneous regime of binary polymer blends, the principle of time-temperature superposition (TTS) holds for both G' and G". However, in the pretransitional regime, the thermorheological complexities set in, which are shown as the breakdown of TTS for both G' and G" , enhanced elasticity and prolonged
relaxation time; and G are more sensitive than G" to phase separation. (2) A single dynamic temperature ramp test is adequate in determining both the binodal and spinodal phase separation temperatures. (3) The critical composition and temperature of PMMA/SAN is 56/44 and 184#, respectively. The thermodynamic interaction parameter, %h, between PMMA and SAN segments, is correlated with temperature as x_(b)(T) =0.017-6.442/T . It was extrapolated, according to this equation, to obtain x_(b) at the room temperature, equal to -0.0046, which is near to the value, X> 0.01, which was determined using SANS by other researchers.
2. By incorporating the nucleation and growth phase separation process into the simplified Palierne emulsion model, the binodal phase separation kinetics of PMMA/SAN(80/20) blend and the effect of linear dynamic rheological measurement on the spinodal phase separation process of PMMA/SAN(56/44) were examined in Chapter 4. It has been found that: (1) The delay time of binodal phase separation, similar to that of spinodal phase separation, also exists in binary polymer blends. (2) In theG'- Time curves at a series of low frequencies, the dependence ofG'on time becomes weaker with increasing frequencies; and G'increases rapidly in the initial stage of phase separation, then increases slowly with time. (3) The linear dynamic rheological measurements can influence the evolution of the co-continuous morphology that is formed by spinodal phase separation. Therefore, the dynamic rheological measurements may be not suitable for the examination of spinodal phase separation kinetics. (4) The growth index of the dispersed domains in PMMA/SAN(80/20) mixture is 0.366 which is slightly larger than 1/3 correspo
引文
[1] Fower M E, Barlow J W, Paul D R. Polymer, 1987,28, 1177
[2] Kim E, Kramer E J, Wu W C, et al. Polymer, 1994,35, 5706
[3] Hsu W P. J Appl Polym Sci, 1999,74,2894
[4] Cameron N, Cowie J M G Ferguson R, et al. Europ Polym J, 2002,38,597
[5] Wu G, Miura T, Asai S, et al. Polymer, 2001,42,3271
[6] Feng H, Ye C, Feng Z. Polym J, 1996,28,661
[7] Polios I S, Soliman M, Lee C, et al. Macromolecules, 1997,30,4470
[8] Spies C, Gehrke P. Macromolecules, 1997,30,1701
[9] Schafer R, Zimmermann J, Kressler J, et al. Polymer, 1997,38,3745
[10] Svoboda P, Ougizawa T, Inoue T, et al. Macromolecules, 1997,30,1973
[11] Floudas Q Pakula T, Fischer E W. Acta Polym, 1994,45,176
[12] Bates FS,Roselale J A, Fredrickson G A. J Chem Phys, 1990,92,6255
[13] Hahn K, Schmitt B J, Kirschey M, et al. Polymer, 1992, 33, 5150
[14] Song M, Jiang B. Polymer, 1992,33, 1445
[15] Maruta J, OhnagaT, Inoue T. Macromolecules, 1993,26,6386
[16] Rojanapitayakorn P, Thongyai S, Higgins J S, et al. Polymer, 2001,42,3475
[17] de Gennes P G J Chem Phys, 1980,72,4756
[18] Utracki L A. Polymer Alloys and Blends. New York: Carl Hanser, 1989, P131
[19] Onogi S. Rheology for Chemists. Tokyo: Kagaku Dojin, 1982, P53
[20] Utracki LA. Polym Eng Sci, 1983,23,602
[21] Yanovsky Y G Polymer Rheology: Theory and Practice. London: Chapman & Hall, 1993, P112
[22] 郑强,赵铁军。材料研究学报,1998,12,225
[23] Ferry J D. Viscoelastic Properties of Polymers. NewYork: Wiley, 1980, P56
[24] Doi M, Edward S F. The Theory of Polymer Dynamics. London: Clarendon Oxford, 1986, P218
[25] Rouse P E. J Chem Phys, 1953,21,1272
[26] Han C D, Jhon M S. J Appl Polym Sci, 1986,32,3809
[27] Onogi S, Masuda T, Kitagawa K. Macromolecules, 1970,3, 116
[28] Kim J K. PhD Dissertation, Polytechnic University, Brooklyn, 1990
[29] Han C D, Kim J K. Macromolecules, 1989,22,4292
[30] Prest WM, Porter R S. J Polym Sci, Part A: Polym Chem, 1972, 10, 1639
[31] Araujo MA,Stadler R. Makromol Chem, 1988,189,2169
[32] Brekner M J,Cantow H J, Schneider HA. Polym Bull, 1985, 14, 17
[33] Irving J B. Viscosities of Binary Liquid Mixtures: A Survey of Mixture Equations. National Engnieering Laboratory: East Kilbridge, Glasgow, U.K., 1977
[34] Wu S. Polymer, 1987,28,1144
[35] Aoki Y, Tanaka T. Macromolecules, 1999,32,8560
[36] Friedrich C, Schwarzwalder C, Riemann R-E. Polymer, 1996, 37,2499
[37] Mertsch R, Wolf B A. Ber Bunsen-Ges Phys Chem, 1994,98,1275
[38] Vlassopoulos D, Koumoutsakos A, Anastasiadis S H. J Rheol, 1997,41,739
[39] KapnistosM, Hinichs A, et al. Macromolecules, 1996,29,7155
[40] Han C D, Lem K W. Polym Eng Rev, 1982, 2, 135
[41] Han C D, Kim J K. Polymer, 1993,34,2533
[42] Nesarikar A R. Macromolecules, 1995,28,7202
[43] Mazich K A, Carr S H. J Appl Phys, 1983,54,5511
[44] Ajji A, Choplin L, Prudhomme R E. J Polym Sci, Polym Phys Ed, 1991,29,1573
[45] Stadler R,Freitas L, Krieger V, et al. Polymer, 1988,29,1643
[46] Chung C I, Griesbach, Young L J Polym Sci, Polym Phys. Ed, 1980,18, 1237
[47] Gouinlock E, Porter R S. Polym Eng Sci, 1977,17,534
[48] Widmayer J M, Meyer G C. J Polym Sci, Polym Phys Ed, 1980,18,2217
[49] Bates F S. Macromolecules, 1984,17,2607
[50] Bates F S. Macromolecules, 1985,18,525
[51] Bates F S, Hartney M A. Macrmolecules, 1985,18,2478
[52] Masuda T, Ohta Y, Morikawa A, et al. J Soc Rheol Japan, 1987, 15,40
[53] Ohta Y, Morikawa A, Takigawa T, et al. J Soc Rheol Japan, 1987,15,141
[54] Ohta Y, Kojima T, Takigawa T, et al. J Rheol, 1987,31,711
[55] Masuda T, Takigawa T, Kojima T, et al. J Rheol, 1989,33,469
[56] Kim J, Han C D. Macromolecules, 1989,22,383
[57] Fredrickson G H, Larson R G J Chem Phys, 1987, 86,1553
[58] Fredrickson G H, Larson R G Macromolecules, 1987,20,1897
[59] Fredrickson G H. J Chem Phys, 1986,85,5306
[60] Wolf B A. Macromolecules, 1984,17,615
[61] Horst R, Wolf B A. Macromolecules, 1993,26, 5676
[62] Chopra D, Vlassopoulos D. J Rheol, 1998,42,1227
[63] Han C D, Chung C I. J Appl Polym Sci, 1985,30,4431
[64] Stadler R, Araujo M A. Makromol Chem Makromol Symp, 1990,38,243
[65] Mani S, Malone M F, Winter H H. J Rheol, 1992,36,1625
[66] Takahashi Y, Suzuki H, Nakagawa Y, et al. Polym Inter, 1994,34,327
[67] Brekner M, Cantow H, Schneider H. Polym Bull, 1985,14,17
[68] Ajji A, Prud'homme R E. J Polym Sci, Polym Phys, 1988,26,2279
[69] Wu S. J Polym Sci, Polym Phys, 1987,25, 557
[70] Yang H H, Han C D, Kim J K. Polymer, 1994,35,1503
[71] Han C D,Yang H H.J Appl Polym Sci, 1987,33,1199
[72] Aoki Y, Arendt O. J Appl Polym Sci. 2001, 82,2037
[73] Pathak J A, Colby R H, Stadler R, et al. Macromolecules, 1998,31,8988
[74] Zheng Q, Du M, Yang B, et al. Polymer, 2001,42,5743
[75] Zheng Q,Araki O,Takahashi M,et al. Polym Preprints, Japan, 1994,43,1024
[76] Zheng Q, Araki O, Masuda T. Chem J Chinese Universities, 1998,19,1329
[77] Zheng Q, Takahashi M, Masuda T. Chem J Chinese Universities, 1999,20,969
[78] Chopra D, Kontopoulou M, Vlassopoulos D, et al. Rheol Acta, 2002,41,10
[79] Pathak J A, Gurp M V. J Appl Polym Sci, 2000,78,1245
[80] Jeon H S,Nakatani A I, Han C C,et al.Macromolecules,2000, 33,9732
[81] ColbyRH. Polymer, 1989,30,1275
[82] Kapnistos M, Vlassopoulos D, Anastasiadis S H. Europhys Lett, 1996,34,513
[83] Vlassopoulos D. Rheol Acta, 1996,35,556
[84] Kim J K, Lee H H, Han C D, et al. Macromolecules, 1998,31,8566
[85] Dumoulin M M, Utracki L A, Carreau P J. In: Utracki L A(ed) Two-phase Polymer Systems. Manser, New York.
[86] Carreau P J, Bousmina M, Ajji A. Pacific Polymer Science 3. Springer, Berlin Heidelberg New York, P25-40
[87] Macmaster L P. Adv Chem Ser, 1975, 142,43
[88] Han C D. Multiphase Flow in Polymer Processing. Academic: New York, 1981
[89] Vincker I, Moldenaers P, Mewis J. J Rheol, 1996,40, 613
[90] Graebling D, Muller R. J Rheol, 1990,34, 193
[91] Palieme J F. Rheol Acta, 1990,29,204
[92] Graebling D, Muller R, Palieme J F. Macromolecules, 1993,26,320
[93] Vinckier I, Laun H M. Rheol Acta, 1999,38,274
[94] Sigga E D. Phys Rev A, 1979,20,595
[95] Doi M, Ohta T. J Chem Phys, 1991,95, 1242
[96] Kim J K, Son H W, Lee Y, et al. J Polym Sci, Polym Phys, 1999,37,889
[97] Zhang Z L, Zhang H D, Yang Y L, et al. Macromolecules, 2001,34,1416
[98] Meijer H E H, Lemstra P M. Makromol Chem, Makromol Symp, 1988, 16,113
[99] Hales B, Bertrand G L, Hepler L G J Phys Chem, 1966,70,3970
[100] Synder R B, Eckert C A. J Chem Eng Data, 1973,18,282
[101] Tveekrem J L, Jacobs D T. Phys Rev A, 1983,27,2773
[102] Gritsenko O T, Nesterov A E. Eur Polym J, 1991 , 27, 455
[103] NesterovAE, Lipatov Y S, Horichko V V, et al. Polymer, 1992, 33, 619
[104] LipatovYS, Nesterov A E. Polym Eng Sci, 1992,32, 1261
[105] Karim A, Liu D W, Douglas J F, et al. Polymer, 2000, 41 , 8455
[106] Lipatov Y S, Nesterov A E, Ignatova T D, et al. Polymer, 2002, 43, 875
[107] Wu S H. Polym Sci, Polym Phys Ed, 1987, 25, 2511
[108] Pierre W. Phys Rev Lett, 1991, 66, 3000
[109] 孔祥明,谢绪明,高宁,张增民。高分子学报,1999,(6) ,752
[110] 刘耀东,孔祥明,谢绪明。高分子学报,2002,(6) ,824
[1] Davies R O, Jones G O. Adv Phys, 1953, 2, 370
[2] Hodge IM. J Non-Cryst Solids, 1994, 169, 211
[3] Struik L C E. Physical Aging in Amorphous Polymers and Other Materials. Amsterdam: Elsevier, 1978
[1] Naito K, Johson G E, Allara D L, et al. Macromolecules, 1978, 11, 1260
[2] Schafer R, Zimmermann J, Kressler J, et al. Polymer, 1997, 38, 3745
[3] Mcbriety V J, Douglas D C, Kwei T K. Macromolecules, 1978, 11 , 1265
[4] Feng H, Ye C, Feng Z. Polym J, 1996, 28, 661
[5] Stein V D J, Jung R H, Illers K H, et al. Angew Makromol Chem, 1974, 36, 89
[6] Kressler J, Higashida N, Inoue T, et al. Macromolecules, 1993, 26, 2090
[7] Suess M, Kressler J, Kammer H W. Polymer, 1987, 28, 957
[8] Ikawa K, Uemura A, Hosoda S, et al. Polym J, 1991, 23, 1291
[9] Song M, Jiang B. Polymer, 1992, 33, 1445
[10] Maruta J, Ohnaga T, Inoue T. Macromolecules, 1993, 26, 6386
[11] Jelenic J, Kirste R G, Schmitt B J, et al. Makromol Chem, 1979, 180, 2057
[12] Hahn K,Schmitt B J, Kirschey M, et al. Polymer, 1992,33, 5150
[13] Fower M E, Barlow J W, Paul D R. Polymer, 1987, 28, 1177
[14] Fower M E, Barlow J W, Paul D R. Polymer, 1987, 28, 2145
[15] Kim E, Kramer E J, Wu W C, et al. Polymer, 1994, 35, 5706
[16] Song M, Hammiche A, Pollock H M, et al. Polymer, 1995, 36, 3313
[17] Hsu W P. J Appl Polym Sci, 1999, 74, 2894
[18] Cameron N, Cowie J M Q Ferguson R, et al. Europ Polym J, 2002, 38, 597
[19] Madbouly S A, Ougizawa T, Inoue T. Macromolecules, 1999, 32, 5631
[20] Hong Z, Shaw M T, Weiss A. Macromolecules, 1998, 6211
[21] Hong Z, Shaw M T, Weiss RA. Polymer, 2000,5895
[22] Paul D R, Newman S. Polymer Blends. Academic Press: New York, 1978, Vol. 1
[23] Pfeng JL, Keskkula H, Barlow J W, et al. Macromolecules, 1985, 18,1937
[24] Wu S. Polymer, 1987,28,1144
[25] Wu S. J Polym Sci, Polym Phys Ed, 1987,25,2511
[26] Han C D, Kim J K. Macromolecules, 1989,22, 1914
[27] Han C D, Kim J K. Macromolecules, 1989,22,4292
[28] Yang H H, Han C D, Kim J K. Polymer, 1994,35,1503
[29] Pathak J A, Colby R H, Stadler R, et al. Macromolecules, 1998,31,8988
[30] Aoki Y, Tanaka T. Macromolecules, 1999,32,8560
[31] Zheng Q, Du M, Yang B, et al. Polymer, 2001,42,5743
[32] Kapnistos M, Hinichs A, et al. Macromolecules, 1996,29,7155
[33] Chopra D, Vlassopoulos D. J Rheol, 1998,42,1227
[34] Chopra D, Kontopoulou M, Vlassopoulos D, et al. Rheol Acta, 2002,41,10
[35] Jeon H S, Nakatani A I, Han C C, et al. Macromolecules, 2000,33,9732
[36] 顾国芳,浦鸿汀编着。聚合物流变学。上海:同济大学出版社,2000。
[37] Ferry J D. Viscoelastic Properties of Polymers, 3rd ed.. NewYork: Wiley, 1980.
[38] Onogi S, Masuda T, Kitagawa K. Macromolecules, 1970,3,116
[39] Stadler R, Freitas L, Krieger V, et al. Polymer, 1988, 29, 1643
[40] Ajji A, Prud'homme R E. J Polym Sci, Polym Phys, 1988,26,2279
[41] Han C D, Kim J K. Polymer, 1993, 34,2533
[42] Kim J, Han C D. Macromolecules, 1989,22,383
[43] Zheng Q, Araki O, Takahashi M, et al. Polym Preprints, Japan, 1994,43,1024
[44] Zheng Q,ArakiO, Masuda T.ChemJ Chinese Universities, 1998,19, 1329
[45] Zheng Q, Takahashi M, Masuda T. Chem J Chinese Universities, 1999,20,969
[46] Fredrickson G H, Larson R G J Chem Phys, 1987,86,1553
[47] Fredrickson G H, Larson R G Macromolecules, 1987,20,1897
[48] Fredrickson G H. J Chem Phys, 1986,85,5306
[49] Wolf B A. Macromolecules, 1984, 17,615
[50] Horst R, Wolf B A. Macromolecules, 1993,26,5676
[51] Nesarikar A R. Macromolecules, 1995,28,7202
[52] Han C D, Yang H H. J Appl Polym Sci, 1987,33,1199
[53] Han C D, Baek D H, Kim J K, et al. Macromolecules, 1995,28,5043
[54] Dumoulin M M, Utracki L A, Carreau P J. In: Utracki L A(ed) Two-phase Polymer Systems. Hanser, New York.
[55] Kapnistos M, Vlassopoulos D, Anastasiadis S H. Europhys Lett, 1996,34,513
[56] Vlassopoulos D. Rheol Acta, 1996, 35, 556
[57] Vlassopoulos D, Koumoutsakos A, Anastasiadis S H. J Rheol, 1997, 41, 739
[58] Bates FS. Macromolecules, 1984, 17,2607
[59] Ajji A, Choplin L. Macromolecules, 1991,24, 5221
[60] de Gennis P G Scaling Concepts in Polymer Physics. Cornell University Press: Ithaca, New York, 1979
[61] Binder K. J Chem Phys, 1983, 79, 6387
[62] Graebling D, Muller R. J Rheol, 1990, 34, 193
[63] Graebling D, Muller R. J, Palierne J F. Macromolecules, 1993, 26, 320
[64] Roovers J, Toporowski P M. Macromolecules, 1992, 25, 3454
[65] Roovers J, Wang F. J Non-Crystalline Solids, 1994, 172-174, 698
[66] Karatasos K, Vlachos G, Vlassopoulos D, et al. J Chem Phys, 1998, 108, 5997
[67] Utracki LA. Polymer alloys and blends: thermodynamics and rheology. Hanser, New York
[68] Friedrich C, Schwarzwalder C, Riemann R E. Polymer, 1996, 37, 2499
[69] Kwei T K. J Polym Sci, Polym Lett Ed, 1984, 22, 307
[70] Hale A, Bair H E. Polymer Blends and Block Copolymers. In: Turi A(ed) Thermal characterization of polymeric materials, 2nd edn, vol 1 . Academic Press, N Y.
[1] QiuF, Peng G,GinzburgV V, et al.J Chem Phys, 2001, 115,3779
[2] Gunton J D, et al. Phase Transition and Critical Phenomena. London: Academic, 1983, vo18.
[3] Hashimoto T, Izumitani T. Polym Prepr, 1985, 26, 66
[4] Hashimoto T, Izumitani T, Takenaka M. J Chem Phys, 1985, 83, 3694
[5] Hashimoto T, Takenaka M, Izumitani T. J Chem Phys, 1990, 92, 4566
[6] 宋墨,粱好均,姜炳政。高分子学报,1990,2,174
[7] Song M, Liang H, Jiang B. Polym Bull, 1990, 23, 615
[8] Hashimoto T, Itakura M, Shimidzu N. J Chem Phys, 1986, 85, 6773
[9] Inaba N, Sato K, Susuki S, et al. Macromolecules, 1986, 19, 1690
[10] Nojima S, Ohyama Y, Yamaguchi M, et al. Polym J, 1982, 14, 907
[11] Hashimoto T, Sasaki K, Kawai H. Macromolecules, 1984, 17, 281
[12] Lifshitz I M, Slyozov V V. J Phys Chem Solids, 1961 , 19, 35
[13] Grant M, Elder K. Phys Rev Lett, 1999, 82, 14
[14] Furukawa H. Phys Rev A, 1985, 31 , 1103
[15] Sigga E D. Phys Rev A, 1979, 20,595
[16] Williams K, Dawe R A. J Colloid Interface Sci, 1987, 81,117
[17] Lee B P, Douglas J F, Glotzer S C. PRE, 1999, 60, 5812
[18] Karim A, Douglas J F, Nisato G, et al. Macromolecules, 1999, 32, 5917
[19] Bray A J. Adv Chem Phys, 1994,43,357
[20] Miguel M S, Grant M, Gunton J D. Phys Rev A, 1985,31,1001
[21] Farrell J E, Vails O T. Phys Rev B, 1990,42,2353
[22] Osborn W R, Orlandini E, Swift M R, et al. Phys Rev Lett, 1995,75,4031
[23] Bastea S, Lebowitz J L. Phys Rev E, 1995,52,3821
[24] Lookman T, Wu Y, Alexander F J, et al. Phys Rev E, 1996,53,5513
[25] Leptoukh G, Strickland B, Roland C. Phys Rev Lett, 1995,74,3636
[26] Grant M, Elder K R. Phys Rev Lett, 1999,82,14
[27] Ikawa K, Uemura A, Hosoda S, et al. Polym J, 1991,23, 1291
[28] Song M, Jiang B. Polymer, 1992,33,1445
[29] Polios I S, Solirnan M, Lee C, et al. Macromolecules, 1997,30,4470
[30] Mani S, Malone M F, Winter H H. J Rheol, 1992,36,1625
[31] Kim J K, Son H W, Lee Y, et al. J Polym Sci, Polym Phys, 1999,37, 889
[32] Einstein A. Ann Phys, 1906, 19,289
[33] Einstein A. Ann Phys, 1911,34,591
[34] Taylor G I. Pro R Soc London, 1932, A132,41
[35] Taylor G I. Pro R Soc London, 1934, A146, 501
[36] Frolich H, Sack R. Pro R Soc London, 1946, A185,415
[37] Oldroyd J G Proc R Soc London, 1953, A218,122
[38] Oldroyd J G Proc R Soc London, 1955, A232,567
[39] Kemer E H. Proc Phys Soc, 1956,69,808
[40] Uemura S, Takayanagi M J. J Appl Polym Sci, 1966, 10, 118
[41] Schowalter W R, Chaffey C E, Brenner H. J Colloid Interface Sci, 1968,26,152
[42] Dickie R A. J Appl Polym Sci, 1973, 17, 45
[43] Choi S J, Schowalter W R. Phys Fliuds, 1975,18,420
[44] Palieme J F. Rheol Acta, 1990,29,204
[45] Jeon H S, Nakatani A I, Han C C, et al. Macromolecules, 2000,33,9732
[46] Vinckier I, Laun H M. Rheol Acta, 1999, 38,274
[47] Graebling, D, Muller R. J, Palieme J F. Macromolecules, 1993,26,320
[48] Gramespacher H, Meissner J. J Rheol, 1992,36,1127
[49] Vinckier I, Laun H M. Rheol Acta, 1999, 38,274
[50] Wu S. Polymer, 1987,28, 1144
[51] Friedrich C, Gleinser W, Korat E, et al. J Rheol, 1995, 39,1411
[52] Kapnistos M, Hinrichs A, Vlassopoulos D, et al. Macromolecules, 1996,29,7155
[53] Matsumoto T, Hori N, Takahashi M. Langmuir, 1996, 12, 5563
[54] Graebling D, Muller R. J Rheol, 1990,34,193
[55] Bank M, Leffingwell J, Thies C. J Polym Sci, Part A-2, 1972, 10, 1097
[56] Binder K, Frisch H L, Jackie J. J Chem Phys, 1986, 85, 1505
[57] Clarice N, Mcleish TCB, Pavawongsak S, et al. Macromolecules, 1997, 30, 4459
[58] Gerard H, Higgins J S, Clarke N. Macromolecules, 1999, 32, 5411
[59] Rojanapitayakom P, Thongyai S, Higgins J S, et al. Polymer, 2001 , 42, 3475
[60] Pincus P. J Chem Phys, 1981, 75, 1996
[61] Binder K. J Chem Phys, 1983, 79, 6387
[62] Ohta T, Nozaki H, Doi M. J Chem Phys, 1990, 93, 2664
[63] Ajji A, Choplin L, Prudhomme R E. J Polym Sci, Polym Phys Ed, 1991, 29, 1573
[64] Vlassopoulos D. Rheol Ada, 1996, 35, 556
[65] Vlassopoulos D, Koumoutsakos A, Anastasiadis S H. J Rheol, 1997, 41, 739
[66] Weis C, Leukel J, Borkenstein K, et al. Polym Bull, 1998, 40, 235
[67] Zhang Z L, Zhang H D, Yang Y L, et al. Macromolecules, 2001, 34, 1416
[68] Macmaster L P. Adv Chem Ser, 1975, 142, 43
[1] Meijer H E H, Lemstra P M. Makromol Chem, Makromol Symp, 1988, 16, 113
[2] Hales B, Bertrand G L, Hepler L G J Phys Chem, 1966, 70, 3970
[3] Synder R B, Eckert C A. J Chem Eng Data, 1973, 18,282
[4] Tveekrem J L, Jacobs D T. Phys Rev A, 1983, 27, 2773
[5] Karim A, Liu D W, Douglas J F, et al. Polymer, 2000, 41, 8455
[6] Lipatov Y S, Shilov V V, Kovemik V V. Rep Acad Sci Ukraine, B 1986, 1, 41
[7] Nesterov A E, Lipatov Y S, Horichko V V, et al. Polymer, 1992, 33,619
[8] Nesterov A E, Lipatov Y S, et al. Rep Acad Sci USSR, 1988, 299, 656
[9] Lipatov Y S, Nesterov A E. Thermodynamics of Polymer Blends. Lancaster-Basel: Technomoc, 1997
[10] Lipatov YS, Nesterov A E. Polym Eng Sci, 1992,32, 1261
[11] Nesterov A E, Lipatov Y S, et al. Macromol Chem Phys, 1998, 199, 2609
[12] Nesterov A E, Lipatov Y S, Ignatova T D. Eur Polym J, 2001 , 37, 281
[13] NesterovAE, Lipatov YS. Polymer, 1999,40, 1347
[14] Lipatov Y S. Polym Yearbook, 1994, 11, 111
[15] Kalfoglou N K. J Appl Polym Sci, 1986, 32, 5247
[16] Feng H, Ye C, Feng Z. Polym J, 1996, 28, 661
[17] Schuster R H, Issel H M, Peterseim V I. Rubber Chem Technol, 1996, 69, 769
[18] Premphet K, Horanont P. Polymer, 2000, 41 , 9283
[19] Sumita M,Sakata K,Asai S et al. Polym Bull, 1991,25,265
[20] Hobbs S Y, Dekkers M E J, Watkins V H. Polymer, 1988, 29, 1598
[21] Wu S. Polymer Interface and Adhesion, Vol 1, New York: Marcel Dekker, 1982
[22] Wu S. Polym Eng Sci, 1987,27,335
[23] Pukanszky B, Fekete E. Adv Polym Sci, 1999,139,109
[24] Han C D, Kim J K. Polymer, 1993,34,2533
[25] Kapnistos M, Hinichs A, et al. Macromolecules, 1996,29,7155
[26] Ajji A, ChoplinL, Prudhomme RE. J Polym Sci, Polym Phys Ed, 1991,29,1573
[27] Zheng Q, Du M, Yang B, et al. Polymer, 2001,42,5743
[28] Kapnistos M, Vlassopoulos D, Anastasiadis S H. Europhys Lett, 1996,34,513
[29] Vlassopoulos D. Rheol Acta, 1996,35,556
[30] Kim J K, Lee H H, Han C D, et al. Macromolecules, 1998,31,8566
[31] Scherbakoff N, Ishida H. J Adhes, 1997,64,203
[32] Vignaux-Nassiet V, AllAl A, Montfort J P. Eur Polym J, 1998,34,309
[33] Scheutjens JMHM, Fleer G J. J Phys Chem, 1979,83,122
[34] Doi M, Kuzuu. J Polym Sci, Polym Lett Ed, 1980,18,775
[35] de Gennes P G J Phys, 1975,36,1199
[36] Pearson D S, Helfand. Macromolecules, 1987,20,148
[38] Ren J, Silva AS, Krishnamoorti R. Macromolecules, 2000,33,3739
[39] Friedrich C, Scheuenpflug W, Neuhausler S, et al. J Appl Polym Sci, 1995,57,499
[40] Krishnamoorti R, Vaia R A, Giannelis E P. Chem Mater, 1996,8: 1728
[41] Enikolopyan N S, Fridman M L, Stalnova I U, et al. Adv Polym Sci, 1990,96:1
[42] Zheng Q, Du M, Yang B, et al. Polymer, 2001, 42, 5743
[43] Kapnistos M, Hinichs A, et al. Macromolecules, 1996,29, 7155
[44] Stadler R, Freitas L, Krieger V, et al. Polymer, 1988,29,1643
[45] Ajji A, Prud'homme R E. J Polym Sci, Polym Phys, 1988,26,2279
[46] Kapnistos M, Hinichs A, et al. Macromolecules, 1996,29, 7155
[47] Fredrickson G H, Larson R G J Chem Phys, 1987,86,1553
[48] Fredrickson G H, Larson R G Macromolecules, 1987,20, 1897
[49] Fredrickson G H. J Chem Phys, 1986,85,5306
[50] Onogi S, Matsumoto T. Polym Eng Rev, 1981, 1,45
[51] Aranguren M I, Mora E, DeGroot Jr J V, et al. J Rheol, 1992,36,1165
[52] Vlassopoulos D. Rheol Acta, 1996, 35,556
[53] Vlassopoulos D, Koumoutsakos A, Anastasiadis S H. J Rheol, 1997,41,739
[54] Dumoulin M M, Utracki L A, Carreau P J. In: Utracki L A(ed) Two-phase Polymer Systems. Hanser, New York.
[55] Silva A S, Tse M F, Krishnamoorti R, et al. J Chem Phys, 2001,115,7166
[56] Lipatov Y S, Nesterov A E, Ignatova T D, et al. Polymer, 2002,875
[57] Leblanc J L, Stragliati B. J Appl Polym Sci, 1997, 63, 959
[58] Leblanc J L. Prog Polym Sci, 2002, 27, 627
[59] Duke J, Taft W K, Kolthoff I M. Rubber Chem Technol, 1952, 25, 500
[60] Kraus G, Gruver J T. Rubber Chem Technol, 1968, 41, 1256
[61] Scheutjens JMHM, Fleer G J. Eff Polym Discuss Prop, London, e.a. 1982, 145-166, Discuss 166-168
[62] Lipatov Y S, Feinerman A, Todosijchuk T, et al. J Colloid Interface Sci, 2000, 228, 114
[63] Fox T G Bull Am Phys Soc, 1956, 1, 123
[64] Cohen-Addad J P. Polymer, 1989, 30, 1820
[65] Cohen-Addad J P. Polymer, 1992, 33, 2762
[1] Fried J. Polymer additives, blends and composites. Polymer Science and Technology. New Jersey: Prentice Hall, 1995, P251
[2] Zaiken A E, Mindubaev R Y, Arhireev V P. Colloid J, 1999, 61 , 459
[3] Gunton J D, San Miguel M, Sahni P. Phase Transition and Critical Phenomena. London: Academic Press, 1983, vo18.
[4] Elder K R, Rogers T M, Desai R C. Phys Rev B, 1988, 38, 4725
[5] Bray A J. Adv Phys, 1994, 43, 357
[6] Puri S, Frisch H L. J Phys Cond Matte, 1997, 9, 2109
[7] Jones R A L, et al. Phys Rev Lett, 1991, 66, 1326
[8] Xie R,Karim A, Douglas JF.et al. Phys Rev Lett, 1998, 81, 1251
[9] Williams K, Dawe R A. J Colloid Interface Sci, 1987, 81 , 117
[10] Liu A J, et ql. Phys Rev Lett, 1990, 65, 1897
[11] Guenoun P, et al. Phys Rev Lett, 1990, 65, 2406
[12] Wiltzius P, Cumming A, Phys Rev Lett, 1991 , 66, 3000
[13] Bruder F, Brenn R. Phys Rev Lett, 1992, 69, 624
[14] Bodensohn J, Goldberg WI. Phys Rev A, 1992,46,5084
[15] Pierre W. Phys Rev Lett, 1991, 66, 3000
[16] 孔祥明,谢绪明,高宁,张增民。高分子学报,1999,(6) .752
[17] 刘耀东,孔祥明,谢绪明。高分子学报,2002,(6) ,824
[18] Lipatov YS.Nesterov A E. Polym Eng Sci, 1992,32, 1261
[19] Nesterov A E, Lipatov Y S, Horichko V V, et al. Polymer, 1992,33,619
[20] Tanaka H, Lovinger A J, Davis D D. Phys Rev Lett, 1994, 72, 2581
[21] Ginzburg V V, Qiu F, Paniconi M, et al. Phys Rev Lett, 1999, 82, 4026
[22] Ginzburg V V, Peng G, Qiu F, et al. Phys Rev E, 1999, 60, 4352
[23] Balazs A C, Ginzburg V V, Qiu F, et al. J Phys Chem B, 2000, 104, 3411
[24] Lifshitz I M, Slyozov V V. J Phys Chem Solids, 1961, 19, 35
[25] Palierne J F. Rheol Acta, 1990, 29, 204
[26] Vignaux-Nassiet V, AllAl A, Montfort J P. Eur Polym J, 1998, 34, 309
[27] Vinckier I, Laun H M. Rheol Acta, 1999, 38, 274
[28] Graebling D, Muller R. J, Palieme J F. Macromolecules, 1993, 26, 320
[29] FriedrichC,Gleinser W,Korat E,et al. J Rheol, 1995,39, 1411
[30] Kapnistos M, Hinrichs A, Vlassopoulos D, et al. Macromolecules, 1996, 29, 7155
[31] Matsumoto T, Hori N, Takahashi M. Langmuir, 1996, 12, 5563
[32] Graebling D, Muller R. J Rheol, 1990, 34, 193
[33] Lipatov Y S, Nesterov A E, Ignatova T D, et al. Polymer, 2002, 43, 875
[34] Clarke N, Mcleish TCB, Pavawongsak S, et al. Macromolecules, 1997, 30, 4459
[35] Pincus P. J Chem Phys, 1981, 75, 1996
[36] Binder K. J Chem Phys, 1983, 79, 6387
[37] Silva A S, Tse M F, Krishnamoorti R, et al. J Chem Phys, 2001 , 115, 7166
[38] Xie X, Matsuoka M, Takemura K. Polymer, 1992, 33, 1996
[39] Xie X, Chen Y, Zhang Z. Macromolecules, 1999, 32, 4424
[40] Xie X, Hu W, Chen Y, et al. Tsinghua Sci Technol, 1996, 1 ,390
[41] 谢绪明,肖天晶,杨勇。高等学校化学学报,1998,19,1864
[42] 肖天晶,谢绪明。功能高分子学报,1996,9,501
[43] Xie X, Xiao T, Zhang Z, et al. J Colloid and Interface Science, 1998, 206, 189
[44] Gubbels F, Blacher S, Vanlathem E, et al. Macromolecules, 1995, 28, 1559
[45] Sumita M, Sakata K, Asai S, et al. Polym Bull, 1991 , 25, 265
[46] Zhang C, Yi X, Yui H, et al. J Appl Polym Sci, 1998, 69, 1813
[47] Cheah K, Forsyth M, Simon G P. J Polym Sci, Polym Phys, 2000, 38, 3106
[49] Calbeg C, Blacher S, Gubbels F, et al. J Phys Appl Phys, 1999, 32, 1517
[50] Zhang C, Han H, Yi X, et al. Compos Interf, 1999, 6, 227
[1] Lipatov Y S. Polymer Yearbook, 1994, 11 , 111
[2] Lipatov Y S. Polymer Reinforcement. Chem Tec Publ, Toronto, 1995
[3] Lipatov Y S. Controlled Interphases in Composite Materials. Elsevier, 1990, P599
[4] Lipatov Y S, Shinfrin V V, Godova E G, et al. Polymer Science USSR, 1989, A31, 1464
[5] Lipatov Y S. Wcience Eng Compos Mater, 1991 , 2, 69
[6] Kwei T K, Radigan H L, Vogel S. Macromolecules, 1977, 10, 157
[7] Goh S H, Siow K S. Thermochimica Acta, 1986, 105, 191
[8] Goh S H, Siow K S, Yap K S. Thermochimica Acta, 1986, 102, 281
[9] Pomposo J A, Calahorra E, Eguiazabal I, et al. Macromolecules, 1993, 26, 2104
[10] Wang Y Y, Chen S A. Polym Eng Sci, 1981, 21, 47
[11] Shah V S, Keitz J D, Paul D R, et al. J Appl Polym Sci, 1986, 32, 3863
[12] Barlow J W, Paul D R. Polym Eng Sci, 1987, 27, 1482
[13] Ameduri B, Prud'homme R E. Polymer, 1988, 29, 1052
[14] Krause S. J Macromol Sci, C 1972, 7, 251
[15] Lipatov YS. J Adhes, 1992, 37, 181
[16] Flory P J. Principles of Polymer Chemistry. Cornell University Press, Ithaca, New York, 1953
[17] Lipatov Y S, Privalko V P. Vysokomolek Soed, B 1984, 26, 257
[18] Lipatov Y S, Sergeeva L M. Adsorption of Polymers. Wiley, 1974
[19] Lipatov Y S, Nesterov A E, Ignatova T D, et al. Polymer, 2002, 43, 875
[20] Nesterov A E, Lipatov Y S, Ignatova T D. European Polym J, 2001 , 37, 281
[21] Lipatov Y S, Shumsky V F, Rosovitsky V F, et al. J Appl Polym Sci, 1993, 47, 941
[22] Nesterov A E, Horicnko V V, Lipatov Y S. Reports Acad Sci USSR, 1988, 299, 656
[23] Gritsenko O T, Nesterov A E. Eur Polym J, 1991 , 27, 455
[24] Meijer H E H, Lemstra P M. Makromol Chem, Makromol Symp, 1988, 16, 113
[25] Nesterov A E, Horichko V V, Lipatov Y S. Makromol Chem Rapid Commun, 1991 , 12, 571
[26] Scheutjens JMHM, Fleer G J. J Phys Chem, 1979, 83, 122
[1] Lee H M, Park O O. J Rheol, 1994, 38, 1405
[2] Doi M, OhtaT. J Chem Phys, 1991, 95, 1242
[3] Guenther G K, Baird D G J Rheol, 1996, 40, 1