▎ 摘　　要

The successful isolation of single-layer graphene sheet has led to tremendous progress in the discovery of new 2D materials including boron nitride, silicene, mxene, phosphorene, and transition metal dichalcogenides. However, the practical applications based on one simple 2D material are still at very early stage. Interfacing electrically and optically active graphene with other 2D materials or crystalline substrate will form a van der Waals heterostructured nanohybrid, which is attracting growing research interest across the disciplines of physics, chemistry, and material science. Such delicate heterostructures can combine the electronic functionality from each individual 2D material, holding great promise for applications in nanoscale electronics and sustainable energy. Computational exploration of electronic functionality in 2D graphene-based van der Waals heterostructures can offer great theoretical insights and design principle that may prove profitable for experimental synthesis and device fabrications. In this review, we highlight recent progress on modeling graphene-based van der Waals nanohybrids using density functional theory-based approach. Particular emphasis will be given on the design of van der Waals heterostructured nanohybrids to modulate stability, stacking geometry, band gap, quantum spin Hall effect, electrical conductivity, optical/friction properties, chemical reactivity, Schottky barrier, carbon dioxide capture, etc. We also comment on the challenges that need to be overcome and outline some interesting research opportunities for future computational exploration of electronic functionality in 2D van der Waals heterostructures. (C) 2016 John Wiley & Sons, Ltd