Graphene nanoscrolls with one-dimensional topological structure obtained by Archimedean-type spirals of graphene, inherit the intrinsic properties of the pristine graphene. They have some unique advantages, including open edges/ends, adjustable internal volume, and diameter. Notably, the accommodation of functionalized components in their open interlayer is potentially a fantastic strategy to promote the epoch-making progress in nanotechnology areas, including energy storage, environmental remediation, biotechnology, and smart devices. However, it could destroy the driving forces for the self-rolling of graphene nanosheets and thus it is still a challenge to prepare functionalized graphene nanoscrolls. Here, based on density functional theory prediction, we reported a feasible method to fabricate graphene oxide nanoscrolls with carbon nanotubes as the template. The method was driven by cation-π interactions, which were caused by metal cations that also acted as the adsorption center. Most importantly, the distinct mechanism and an acidity-dependent rule for the formation of graphene nanoscrolls were identified. Benefiting from the introduced metal cations and the macro three-dimensional hierarchical structure, the produced nanoscroll aerogel exhibited significantly improved adsorption performance toward different organic solvents with the adsorption capacities from 129.9 to 265.7 g g−1. This work demonstrates a simple and efficient strategy to fabricate functionalized component-accommodated graphene nanoscroll, which could find important applications in various fields.
