Tailoring Interfacial Properties in Polymer-Silica Nanocomposites via Surface Modification: An Atomistic Simulation Study

被引:16
作者
Li, Wei [6 ]
Bacova, Petra [1 ]
Behbahani, Alireza F. [1 ]
Burkhart, Craig [2 ]
Polinska, Patrycja [3 ]
Harmandaris, Vagelis [1 ,4 ,5 ]
Doxastakis, Manolis [6 ]
机构
[1] Fdn Res & Technol Hellas, Inst Appl & Computat Math, GR-71110 Iraklion, Greece
[2] Goodyear Tire & Rubber Co, Akron, OH 44305 USA
[3] Goodyear Innovat Ctr Luxembourg, L-7750 Colmar Berg, Luxembourg
[4] Univ Crete, Dept Math & Appl Math, GR-71110 Iraklion, Greece
[5] Cyprus Inst, Computat Based Sci & Technol Res Ctr, CY-2121 Nicosia, Cyprus
[6] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA
关键词
polymer nanocomposites; surface modification; atomistic simulations; grafting density; polymer conformations; interfacial dynamics; CIS-1,4 POLYISOPRENE MELTS; MONTE-CARLO SIMULATION; GLASS-TRANSITION; AMORPHOUS SILICA; FILLER SURFACE; NATURAL-RUBBER; DYNAMICS; REINFORCEMENT; NANOPARTICLES; CHAIN;
D O I
10.1021/acsapm.1c00197
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
Surface modification is an effective way to improve the dispersion of nanofillers in a polymer matrix and tune the interfacial interactions that determine macroscopic properties in polymer nanocomposites. In this work, we present a detailed investigation of silane modification effects on polymer interfacial conformation and dynamic properties through atomistic molecular dynamics simulations, using cis-1,4 polyisoprene (the major component of natural rubber) and amorphous silica substrate as a model system. Industrially relevant modified substrates are constructed with alkylsilane agents grafted at different surface densities. Contrasting systems with the modified substrates to the bare substrate case, we show that silane grafting effectively modulates chain conformations near the silica surface in terms of train, loop, and tail configurations, highlighting the separate effects of silane grafting density and agent chain length. We examine the variation of polymer dynamics in desorption, relaxation, and diffusion, which demonstrates the weakening of dynamic slowing down at the interface due to the silane presence and further exposes the dominant effects of surface train segments on the dynamic properties. Our results offer microscopic information on interfacial behavior while identifying key factors for tailoring interfacial dynamics. These findings provide useful insight into the reinforcement mechanism and serve as a first step toward the rational design of rubber composite materials via chemically detailed computational modeling.
引用
收藏
页码:2576 / 2587
页数:12
相关论文
共 70 条
[1]   Gromacs: High performance molecular simulations through multi-level parallelism from laptops to supercomputers [J].
Abraham, Mark James ;
Murtola, Teemu ;
Schulz, Roland ;
Páll, Szilárd ;
Smith, Jeremy C. ;
Hess, Berk ;
Lindah, Erik .
SoftwareX, 2015, 1-2 :19-25
[2]   DIELECTRIC NORMAL MODE PROCESS IN UNDILUTED CIS-POLYISOPRENE [J].
ADACHI, K ;
KOTAKA, T .
MACROMOLECULES, 1985, 18 (03) :466-472
[3]   CONTIN XPCS: software for inverse transform analysis of X-ray photon correlation spectroscopy dynamics [J].
Andrews, Ross N. ;
Narayanan, Suresh ;
Zhang, Fan ;
Kuzmenko, Ivan ;
Ilavsky, Jan .
JOURNAL OF APPLIED CRYSTALLOGRAPHY, 2018, 51 :205-209
[4]   Multiscale Filler Structure in Simplified Industrial Nanocomposite Silica/SBR Systems Studied by SAXS and TEM [J].
Baeza, Guilhem P. ;
Genix, Anne-Caroline ;
Degrandcourt, Christophe ;
Petitjean, Laurent ;
Gummel, Jeremie ;
Couty, Marc ;
Oberdisse, Julian .
MACROMOLECULES, 2013, 46 (01) :317-329
[5]   Dynamics of polymer segments, polymer chains, and nanoparticles in polymer nanocomposite melts: A review [J].
Bailey, Eric J. ;
Winey, Karen I. .
PROGRESS IN POLYMER SCIENCE, 2020, 105
[6]   Controlling the thermornechanical properties of polymer nanocomposites by tailoring the polymer-particle interface [J].
Bansal, Amitabh ;
Yang, Hoichang ;
Li, Chunzhao ;
Benicewicz, Rian C. ;
Kumar, Sanat K. ;
Schadler, Linda S. .
JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS, 2006, 44 (20) :2944-2950
[7]   Conformations and Dynamics of Polymer Chains in Cis and Trans Polybutadiene/Silica Nanocomposites through Atomistic Simulations: From the Unentangled to the Entangled Regime [J].
Behbahani, Alireza F. ;
Rissanou, Anastassia ;
Kritikos, Giorgos ;
Doxastakis, Manolis ;
Burkhart, Craig ;
Polinska, Patrycja ;
Harmandaris, Vagelis A. .
MACROMOLECULES, 2020, 53 (15) :6173-6189
[8]   Evidence for the shift of the glass transition near the particles in silica-filled elastomers [J].
Berriot, J ;
Montes, H ;
Lequeux, F ;
Long, D ;
Sotta, P .
MACROMOLECULES, 2002, 35 (26) :9756-9762
[9]   Effect of filler particle size on the properties of model nanocomposites [J].
Brown, D. ;
Marcadon, V. ;
Mele, P. ;
Alberola, N. D. .
MACROMOLECULES, 2008, 41 (04) :1499-1511
[10]   Untangling the Effects of Chain Rigidity on the Structure and Dynamics of Strongly Adsorbed Polymer Melts [J].
Carrillo, Jan-Michael Y. ;
Cheng, Shiwang ;
Kumar, Rajeev ;
Goswami, Monojoy ;
Sokolov, Alexei P. ;
Sumpter, Bobby G. .
MACROMOLECULES, 2015, 48 (12) :4207-4219