Citation: Zhao-Yang Wei, Nan-Ying Ning, Ming Tian, Li-Qun Zhang, Jian-Guo Mi. Theoretical Interpretation of Conformation Variations of Polydimethylsiloxane Induced by Nanoparticles[J]. Chinese Journal of Polymer Science, ;2018, 36(4): 505-513. doi: 10.1007/s10118-018-2019-9 shu

Theoretical Interpretation of Conformation Variations of Polydimethylsiloxane Induced by Nanoparticles

Zhao-Yang Wei ^a,b ,
Nan-Ying Ning ^a,b ,
Ming Tian ^a,b,, ,
Li-Qun Zhang ^a,b ,
Jian-Guo Mi ^a,,

a.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
b.
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China

Corresponding author: Ming Tian, tianm@mail.buct.edu.cn Jian-Guo Mi, mijg@mail.buct.edu.cn
Received Date: 23 June 2017
Accepted Date: 11 August 2017
Available Online: 30 November 2017

There has been controversy as to whether the addition of nanoparticles to a polymer melt causes perturbed chain structure of polymers. In this work, the chain conformations of polydimethylsiloxane (PDMS) with addition of polyhedral oligomeric silsesquioxane (POSS) nanoparticles have been studied using a classical density functional approach. Under the strong interactions of POSS-PDMS, the radius of gyration of PDMS in the nanocomposites can either increase or decline depending on particle loading. After adding nanoparticles with larger size or weaker interactions, both the increasing and the declining amplitudes can be largely suppressed. The results provide a deep understanding of chain conformation in polymer nanocomposites.
- Chain conformation,
- Radius of gyration,
- Polymer nanocomposites,
- Density functional theory
1. [1]
  Paul D. R., Robeson L. M.. Polymer nanotechnology:Nanocomposites[J]. Polymer, 2008,49(15):3187-3204. doi: 10.1016/j.polymer.2008.04.017
2. [2]
  Ganesan V.. Some issues in polymer nanocomposites:theoretical and modeling opportunities for polymer physics[J]. J. Polym. Sci., Part B:Polym. Phys., 2008,46(24):2666-2671. doi: 10.1002/polb.v46:24
3. [3]
  Pandey Y. N., Papakonstantopoulos G. J., Doxastakis M.. Polymer/nanoparticle interactions:bridging the gap[J]. Macromolecules, 2013,46(13):5097-5106. doi: 10.1021/ma400444w
4. [4]
  Kumar S. K., Krishnamoorti R.. Nanocomposites:structure, phase behavior, and properties[J]. Annu. Rev. Chem. Biomol. Eng., 2010,1:37-58. doi: 10.1146/annurev-chembioeng-073009-100856
5. [5]
  Allegra G., Raos G., Vacatello M.. Theories and simulations of polymer-based nanocomposites:from chain statistics to reinforcement[J]. Prog. Polym. Sci., 2008,33(7):683-731. doi: 10.1016/j.progpolymsci.2008.02.003
6. [6]
  Genix A. C., Oberdisse J.. Structure and dynamics of polymer nanocomposites studied by X-ray and neutron scattering techniques[J]. Curr. Opin. Colloid Interface Sci., 2015,20(4):293-303. doi: 10.1016/j.cocis.2015.10.002
7. [7]
  Nakatani A., Chen W., Schmidt R., Gordon G., Han C. C.. Chain dimensions in polysilicate-filled poly(dimethyl siloxane)[J]. Polymer, 2001,42(8):3713-3722. doi: 10.1016/S0032-3861(00)00771-0
8. [8]
  Mackay M. E., Tuteja A., Duxbury P. M., Hawker C. J., van Horn B., Guan Z., Chen G., Krishnan R. S.. General strategies for nanoparticle dispersion[J]. Science, 2006,311(5768):1740-1743. doi: 10.1126/science.1122225
9. [9]
  Tuteja A., Duxbury P. M., Mackay M. E.. Polymer chain swelling induced by dispersed nanoparticles[J]. Phys. Rev. Lett., 2008,100(7)077801. doi: 10.1103/PhysRevLett.100.077801
10. [10]
  Tung W. S., Bird V., Composto R. J., Clarke N., Winey K. I.. Polymer chain conformations in CNT/PS nanocomposites from small angle neutron scattering[J]. Macromolecules, 2013,46(13):5345-5354. doi: 10.1021/ma400765v
11. [11]
  Tung W. S., Composto R. J., Clarke N., Winey K. I.. Anisotropic polymer conformations in aligned SWCNT/PS nanocomposites[J]. ACS Macro Lett., 2015,4(9):916-920. doi: 10.1021/acsmacrolett.5b00256
12. [12]
  Nusser K., Neueder S., Schneider G. J., Meyer M., Pyckhout-Hintzen W., Willner L., Radulescu A., Richter D.. Conformations of silica-poly(ethylene-propylene) nano-composites[J]. Macromolecules, 2010,43(23):9837-9847. doi: 10.1021/ma101898c
13. [13]
  Sen S., Xie Y., Kumar S. K., Yang H., Bansal A., Ho D. L., Hall L., Hooper J. B., Schweizer K. S.. Chain conformations and bound-layer correlations in polymer nanocomposites[J]. Phys. Rev. Lett., 2007,98(12)128302. doi: 10.1103/PhysRevLett.98.128302
14. [14]
  Jouault N., Dalmas F., Said S., di Cola E., Schweins R., Jestin J., Boué F.. Direct measurement of polymer chain conformation in well-controlled model nanocomposites by combining SANS and SAXS[J]. Macromolecules, 2010,43(23):9881-9891. doi: 10.1021/ma101682t
15. [15]
  Genix A. C., Tatou M., Imaz A., Forcada J., Schweins R., Grillo I., Oberdisse J.. Modeling of intermediate structures and chain conformation in silica-latex nanocomposites observed by SANS during annealing[J]. Macromolecules, 2012,45(3):1663-1675. doi: 10.1021/ma202308c
16. [16]
  Crawford M., Smalley R., Cohen G., Hogan B., Wood B., Kumar S., Melnichenko Y. B., He L., Guise W., Hammouda B.. Chain conformation in polymer nanocomposites with uniformly dispersed nanoparticles[J]. Phys. Rev. Lett., 2013,110(19)196001. doi: 10.1103/PhysRevLett.110.196001
17. [17]
  Banc A., Genix A. C., Dupas C., Sztucki M., Schweins R., Appavou M. S., Oberdisse J.. Origin of small-angle scattering from contrast-matched nanoparticles:a study of chain and filler structure in polymer nanocomposites[J]. Macromolecules, 2015,48(18):6596-6605. doi: 10.1021/acs.macromol.5b01424
18. [18]
  Jouault N., Crawford M. K., Chi C., Smalley R. J., Wood B., Jestin J., Melnichenko Y. B., He L., Guise W. E., Kumar S. K.. Polymer chain behavior in polymer nanocomposites with attractive interactions[J]. ACS Macro Lett., 2016,5(4):523-527. doi: 10.1021/acsmacrolett.6b00164
19. [19]
  Ganesan V., Khounlavong L., Pryamitsyn V.. Equilibrium characteristics of semiflexible polymer solutions near probe particles[J]. Phys. Rev. E, 2008,78(5)051804.
20. [20]
  Cui J., Li W., Jiang W.. Simulation study of co-assembly of ABC triblock copolymer/nanoparticle into multicompartment hybrids in selective solvent[J]. Chinese J. Polym. Sci., 2013,31(9):1225-1232. doi: 10.1007/s10118-013-1323-7
21. [21]
  Khounlavong L., Ganesan V.. Influence of interfacial layers upon the barrier properties of polymer nanocomposites[J]. J. Chem. Phys., 2009,130(10)104901. doi: 10.1063/1.3079138
22. [22]
  Frischknecht A. L., McGarrity E. S., Mackay M. E.. Expanded chain dimensions in polymer melts with nanoparticle fillers[J]. J. Chem. Phys., 2010,132(20)204901. doi: 10.1063/1.3428760
23. [23]
  Ganesan V., Ellison C. J., Pryamitsyn V.. Mean-field models of structure and dispersion of polymer-nanoparticle mixtures[J]. Soft Matter, 2010,6(17):4010-4025. doi: 10.1039/b926992d
24. [24]
  Vacatello M.. Chain dimensions in filled polymers:an intriguing problem[J]. Macromolecules, 2002,35(21):8191-8193. doi: 10.1021/ma020416s
25. [25]
  Sharaf M. A., Mark J. E.. Monte Carlo simulations on the effects of nanoparticles on chain deformations and reinforcement in amorphous polyethylene networks[J]. Polymer, 2004,45(11):3943-3952. doi: 10.1016/j.polymer.2004.02.073
26. [26]
  Takhulee, Ozisik, Vao-soongnern, V. Monte Carlo simulation of the structure of mono-and bidisperse polyethylene nanocomposites[J]. Chinese J. Polym. Sci., 2015,33(2):275-283. doi: 10.1007/s10118-015-1578-2
27. [27]
  Vogiatzis G. G., Voyiatzis E., Theodorou D. N.. Monte Carlo simulations of a coarse grained model for an athermal all-polystyrene nanocomposite system[J]. Eur. Polym. J., 2011,47(4):699-712. doi: 10.1016/j.eurpolymj.2010.09.017
28. [28]
  Ndoro T. V., Voyiatzis E., Ghanbari A., Theodorou D. N., Böhm M. C., Müller-Plathe F.. Interface of grafted and ungrafted silica nanoparticles with a polystyrene matrix:Atomistic molecular dynamics simulations[J]. Macromolecules, 2011,44(7):2316-2327. doi: 10.1021/ma102833u
29. [29]
  Karatrantos A., Composto R. J., Winey K. I., Clarke N.. Structure and conformations of polymer/SWCNT nanocomposites[J]. Macromolecules, 2011,44(24):9830-9838. doi: 10.1021/ma201359s
30. [30]
  Padmanabhan V., Frischknecht A. L., Mackay M. E.. Effect of chain stiffness on nanoparticle segregation in polymer/nanoparticle blends near a substrate[J]. Macromol. Theory Simul., 2012,21(2):98-105. doi: 10.1002/mats.201100048
31. [31]
  Karatrantos A., Clarke N., Composto R. J., Winey K. I.. Polymer conformations in polymer nanocomposites containing spherical nanoparticles[J]. Soft Matter, 2015,11(2):382-388. doi: 10.1039/C4SM01980F
32. [32]
  Karatrantos A., Clarke N., Kröger M.. Modeling of polymer structure and conformations in polymer nanocomposites from atomistic to mesoscale:a review[J]. Polym. Rev., 2016,56(3):385-428. doi: 10.1080/15583724.2015.1090450
33. [33]
  Hall L. M., Anderson B. J., Zukoski C. F., Schweizer K. S.. Concentration fluctuations, local order, and the collective structure of polymer nanocomposites[J]. Macromolecules, 2009,42(21):8435-8442. doi: 10.1021/ma901523w
34. [34]
  Frischknecht A. L., Padmanabhan V., Mackay M. E.. Surface-induced phase behavior of polymer/nanoparticle blends with attractions[J]. J. Chem. Phys., 2012,136(16). doi: 10.1063/1.4705308
35. [35]
  Ebner C., Saam W., Stroud D.. Density-functional theory of simple classical fluids[J]. I. Surfaces. Phys. Rev. A, 1976,14(6):2264-2273.
36. [36]
  Chandler D., McCoy J. D., Singer S. J.. Density functional theory of nonuniform polyatomic systems[J]. I. general formulation. J. Chem. Phys., 1986,85(10):5971-5976.
37. [37]
  Yu Y. X., Wu J.. Density functional theory for inhomogeneous mixtures of polymeric fluids[J]. J. Chem. Phys., 2002,117(5):2368-2376. doi: 10.1063/1.1491240
38. [38]
  Yu Y. X., Gao G. H., Wang X. L.. Density functional theory study on the structure and capillary phase transition of a polymer melt in a slitlike pore:effect of attraction[J]. J. Phys. Chem. B, 2006,110(29):14418-14425. doi: 10.1021/jp060986k
39. [39]
  Tripathi S., Chapman W.. Microstructure and thermodynamics of inhomogeneous polymer blends and solutions[J]. Phys. Rev. Lett., 2005,94(8)087801. doi: 10.1103/PhysRevLett.94.087801
40. [40]
  Tripathi S., Chapman W. G.. Microstructure of inhomogeneous polyatomic mixtures from a density functional formalism for atomic mixtures[J]. J. Chem. Phys., 2005,122(9). doi: 10.1063/1.1853371
41. [41]
  Yu Y. X., Wu J.. Extended test-particle method for predicting the inter-and intramolecular correlation functions of polymeric fluids[J]. J. Chem. Phys., 2003,118(8):3835-3842. doi: 10.1063/1.1539840
42. [42]
  Yu Y. X., Wu J. Z., You F. Q., Gao G. H.. A Self-consistent theory for the inter-and intramolecular correlation functions of a Hard-Sphere-Yukawa-Chain fluids[J]. Chinese Phys. Lett., 2005,22(1):246-249. doi: 10.1088/0256-307X/22/1/071
43. [43]
  Bymaster A.. "Molecular modeling the microstructure and phase behavior of bulk and inhomogeneous complex fluids"[J]. Thesis, Rice University, 2009.
44. [44]
  Everaers R., Ejtehadi M.. Interaction potentials for soft and hard ellipsoids[J]. Phys. Rev. E, 2003,67(4)041710. doi: 10.1103/PhysRevE.67.041710
45. [45]
  Frischknecht A. L., Curro J. G.. Improved united atom force field for poly(dimethylsiloxane)[J]. Macromolecules, 2003,36(6):2122-2129. doi: 10.1021/ma025763g
46. [46]
  Striolo A., McCabe C., Cummings P. T., Chan E. R., Glotzer S. C.. Aggregation of POSS monomers in liquid hexane:a molecular-simulation study[J]. J. Phys. Chem. B, 2007,111(42):12248-12256. doi: 10.1021/jp071730x
47. [47]
  Rosenfeld Y.. Free-energy model for the inhomogeneous hard-sphere fluid mixture and density-functional theory of freezing[J]. Phys. Rev. Lett., 1989,63(9):980-983. doi: 10.1103/PhysRevLett.63.980
48. [48]
  Hansen, J. P.; McDonald, I., "Theory of Simple Liquids", Academic Press, New York, 1986.
49. [49]
  Jain S., Dominik A., Chapman W. G.. Modified interfacial statistical associating fluid theory:a perturbation density functional theory for inhomogeneous complex fluids[J]. J. Chem. Phys., 2007,127(24)244904. doi: 10.1063/1.2806932
50. [50]
  Chapman W. G., Jackson G., Gubbins K. E.. Phase equilibria of associating fluids[J]. Mol. Phys., 1988,65(5):1057-1079. doi: 10.1080/00268978800101601
51. [51]
  Tree D. R., Muralidhar A., Doyle P. S., Dorfman K. D.. Is DNA a good model polymer?[J]. Macromolecules, 2013,46(20):8369-8382. doi: 10.1021/ma401507f
52. [52]
  Honnell K. G., Curro J. G., Schweizer K. S.. Local structure of semiflexible polymer melts[J]. Macromolecules, 1990,23(14):3496-3505. doi: 10.1021/ma00216a018
53. [53]
  Yethiraj A., Hall C. K.. Monte Carlo simulations and integral equation theory for microscopic correlations in polymeric fluids[J]. J. Chem. Phys., 1992,96(1):797-807. doi: 10.1063/1.462465
54. [54]
  Edwards C. J. C., Richards R. W., Stepto R. F. T., Dodgson K., Higgins J. S., Semlyen J. A.. Studies of cyclic and linear poly(dimethyl siloxanes).14. particle scattering functions[J]. Polymer, 1984,25(3):365-368.
55. [55]
  Arrighi V., Gagliardi S., Dagger A. C., Semlyen J. A., Higgins J. S., Shenton M. J.. Conformation of cyclics and linear chain polymers in bulk by SANS[J]. Macromolecules, 2004,37(21):8057-8065. doi: 10.1021/ma049565w
56. [56]
  Wei Z., Hou Y., Ning N., Zhang L., Tian M., Mi J.. Theoretical insight into dispersion of silica nanoparticles in polymer melts[J]. J. Phys. Chem. B, 2015,119(30):9940-9948. doi: 10.1021/acs.jpcb.5b01399
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