Crumpling and Mechanical Behaviors of Polymer-Grafted Nanosheets*

Understanding the crumpling behavior and mechanical response of polymer-grafted nanosheet materials is of fundamental importance in engineering and technological applications. Here, we report the results of a systematic coarse-grained molecular dynamics simulation study of the crumpling process and compressive properties of polymer-grafted nanosheets at various polymer grafting densities. We find that the degree of crumpling and wrinkling of the nanosheets at equilibrium increases and then decreases with increasing polymer grafting density. By evaluating the evolution of the potential energy of the sheet during the crumpling process, our results show that the grafted polymer chains significantly reduce the adhesion properties of the nanosheets. Notably, the shape descriptor analysis shows less self-folding and self-adhering upon crumpling for sheets with larger grafting density. In addition, the evaluation of the compressive properties of the crumpled system further reveals the enhancement of the mechanical response of the grafted polymers to the crumpled nanosheets. Our findings highlight the critical role of grafted polymer in the crumpling process and mechanical response of nanosheets, which has significant implications for the tailored design of crumpled polymer functionalized nanosheets.