Cavitation, crazing and bond scission in chemically cross-linked polymer nanocomposites

H Zhang and HX Li and FY Hu and WC Wang and XY Zhao and YY Gao and LQ Zhang, SOFT MATTER, 15, 9195-9204 (2019).

DOI: 10.1039/c9sm01664c

It is very important to understand the molecular mechanism of the fracture behavior of chemically cross-linked polymer nanocomposites (PNCs). Thus, in this work, by employing a coarse-grained molecular dynamics simulation we investigated the effect of the cross-link density and the cross-link distribution on it by calculating the void formation and the chemical bond scission. Considering the fracture energy, the optimal fracture properties of PNCs are realized at the moderate cross- link density which results from the competition between the chain slippage induced voids and the bond scission induced voids. Meanwhile, more bond scission occurs on the chain backbone while a high broken percentage of the cross-link bonds appears between chains because of the higher average stress borne by one cross-linked bead than by one other bead. In addition, the number of voids is quantified which first increases and then decreases with the strain at low cross-link density. However, the number of newly formed voids increases again at high cross- link density. Finally, it decreases because of the low rate of bond scission. Furthermore, the chemical bonds are broken at a similar strain for the uniform cross-link distribution while they are broken at any strain for the nonuniform cross-link distribution. The low number of broken bonds induces the disappearance of the second peak of the number of voids with the strain for the nonuniform cross-link distribution. In summary, this work could provide a clear understanding of the fracture mechanism of the chemically cross-linked PNCs on the molecular level.

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