Superior delamination resistant two-dimensional lamellar materials

Abstract

Numerous 2D sheets are generally exfoliated and prevalent to be assembled into macroscopic lamellar materials. However, these highly expected materials still inherit the easy exfoliation of 2D sheets and exhibit severe delamination failure problems, despite their outstanding in-plane performances and functions. Here, we find the increasing stack order of 2D sheets inversely aggravates delamination and uncover the hidden interlayer dissipation as the dominating mechanism. We propose a strong interlayer entanglement toughening strategy to greatly improve the delamination strength of graphene oxide papers by 268%, achieving a superior delamination resistance of benchmark natural nacres. The interlayer disentanglement offers extra dissipative sites to alleviate the stress concentration of the crack tip and suppress the crack propagation. This work provides an effective structural design strategy to resolve the intrinsic delamination problem of 2D lamellar materials, paving the way to realistic applications as structural materials and durable coatings.