From Forces to Assemblies: van der Waals Forces-Driven Assemblies in Anisotropic Quasi-2D Graphene and Quasi-1D Nanocellulose Heterointerfaces towards Quasi-3D Nanoarchitecture.

In the pursuit of advanced functional materials, the role of low-dimensional van der Waals (vdW) heterointerfaces has recently ignited noteworthy scientific interest, particularly in assemblies that incorporate quasi-2D graphene and quasi-1D nanocellulose derivatives. The growing interest predominantly stems from the potential to fabricate distinct genres of quasi-2D/1D nanoarchitecture governed by vdW forces. Despite the possibilities, the inherent properties of these nanoscale entities are limited by in-plane covalent bonding and the existence of dangling π-bonds, constraints that inhibit emergent behavior at heterointerfaces. An innovative response to these limitations proposes a mechanism that binds multilayered quasi-2D nanosheets with quasi-1D nanochains, capitalizing on out-of-plane non-covalent interactions. The approach facilitates the generation of dangling bond-free iso-surfaces and promotes the functionalization of multilayered materials with exceptional properties. However, a gap still persists in understanding transition and alignment mechanisms in disordered multilayered structures, despite the extensive exploration of monolayer and asymmetric bilayer arrangements. In this perspective, we comprehensively review the sophisticated aspects of multidimensional vdW heterointerfaces composed of quasi-2D/1D graphene and nanocellulose derivatives. Further, we discuss the profound impacts of anisotropy nature and geometric configurations, including in-plane and out-of-plane dynamics on multiscale vdW heterointerfaces. Ultimately, we shed light on the emerging prospects and challenges linked to constructing advanced functional materials in the burgeoning domain of quasi-3D nanoarchitecture.