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Focus on the deformation mechanism at the interfacial layer in nano-reinforced polymers: A molecular dynamics study of silica - poly(methyl methacrylate) nano-composite

Bedoui, F. and Jaramillo-Botero, Andres and Pascal, Tod A. and Goddard, William A., III (2021) Focus on the deformation mechanism at the interfacial layer in nano-reinforced polymers: A molecular dynamics study of silica - poly(methyl methacrylate) nano-composite. Mechanics of Materials, 159 . Art. no. 103903. ISSN 0167-6636. doi:10.1016/j.mechmat.2021.103903.

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The effects of nanoparticle size on the “macroscopic” mechanical response and interfacial interaction in the case of model nano-reinforced polymers were investigated using molecular dynamics simulations. Different ensembles, of homogeneous polymer matrices, amorphous silica particle, and their binary mixtures were prepared. The binary mixture was made with silica nano-particle 3 nm in size, embedded in poly (methyl methacrylate) or PMMA polymeric matrix. At the macroscopic scale, the mechanical response of the matrix and nano-composite was evaluated using simulated tensile tests. Interfacial interaction between the NP and the PMMA matrix was qualitatively evaluated using the thermodynamic analysis of nanocomposite systems. Entropy (S) and internal energy (E) were derived from relatively short molecular dynamics trajectories, using the two-phase thermodynamic method (2-PT). The PMMA matrix was decomposed into concentric layers composed of atoms from different polymer chains but located at an equal distance from the center of mass of the silica NP. For both nanocomposite systems, the interface layer of the polymer closest to the silica NP surface exhibited both the lowest entropy and a well-organized structure. Entropy and internal energy patterns were derived from tensile stretched samples. Entropy and internal energy variation on stretched samples revealed the existence of two distinct domains. The first domain deformation was a mixture of internal energy increase and entropy decrease. In the second domain, the deformation mechanism was mostly governed by variations in entropy. These observations will be discussed about polymer – nanoparticle attractivity.

Item Type:Article
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URLURL TypeDescription
Jaramillo-Botero, Andres0000-0003-2844-0756
Pascal, Tod A.0000-0003-2096-1143
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2021 Elsevier Ltd. Received 4 February 2021, Revised 4 May 2021, Accepted 5 May 2021, Available online 8 May 2021. The authors would like to acknowledge the funding support from Région Hauts de France through the INTIM and SENAREO project (RDIPROJFT63 – INV 31) and the helpful support in the computing process from Guy Leon Kaza (Roberval Laboratory FRE-CNRS 2012) and Malik Abbassi (SAS Neoteckno). Caltech received support from DOE (STTR Award DE-SC0017710).
Funding AgencyGrant Number
Région Hauts de FranceRDIPROJFT63 – INV 31
Roberval LaboratoryFRE-CNRS 2012
Department of Energy (DOE)DE-SC0017710
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Record Number:CaltechAUTHORS:20210607-165859382
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109427
Deposited By: Donna Wrublewski
Deposited On:08 Jun 2021 16:08
Last Modified:16 Nov 2021 19:36

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