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Highly Stretchable Polymers: Mechanical Properties Improvement by Balancing Intra‐ and Intermolecular Interactions
Author(s) -
Galant Or,
Bae Suwon,
Silberstein Meredith N.,
Diesendruck Charles E.
Publication year - 2020
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201901806
Subject(s) - intramolecular force , intermolecular force , materials science , polymer , chemical physics , molecular dynamics , elasticity (physics) , covalent bond , polymer chemistry , molecule , computational chemistry , composite material , chemistry , stereochemistry , organic chemistry
The mechanical properties of polymers are highly dependent on the mobility of the underlying chains. Changes in polymer architecture can affect inter‐ and intramolecular interactions, resulting in different chain dynamics. Herein, an enhancement in the mechanical properties of poly(butylmethacrylate) is induced by folding the polymer chains through covalent intramolecular crosslinking (CL). Intramolecular CL causes an increase in intramolecular interactions and inhibition of intermolecular interactions. In both the glassy and rubbery states, this molecular rearrangement increases material stiffness. In the glassy state, this molecular rearrangement also leads to reduced failure strain, but surprisingly, in the rubbery state, the large strain elasticity is actually increased. An intermediate intramolecular CL degree, where there is a balance between intra‐ and intermolecular interactions, shows optimal mechanical properties. Molecular dynamics simulations are used to confirm and provide molecular mechanisms to explain the experimental results.