Simulations of End-Functionalized Polymer Grafted Particles for Additive Manufacturing Applications

Polymer-grafted particles (PGPs) are added to polymeric materials to enhance physical properties while maintaining compatibility with the polymer matrix. Recent work [P. J. Santos, et al., Nature, 2021, 591, 586–591] has shown that end-functionalizing the graft chains on the PGPs can lead to controlled self-assembly into crystalline lattices. These materials offer promising avenues for controlling structure of materials with tailored mechanical, optical, and/or transport properties; however, a fundamental understanding of the mechanisms driving self-assembly of end-functionalized PGPs under different processing conditions is currently lacking. To address this knowledge gap, we use coarse-grained molecular dynamics simulations to study how the end-functional groups on the grafts interact with other end-functional groups as a function of PGP design parameters, namely, graft chain length, particle diameter, and graft chain density. We also show how these materials may be used in additive manufacturing applications and demonstrate how changing the design of an end-functionalized PGP affects grafted layer wetting and stability at the interface between polymer domains.