Controlled Electrochemical Deposition of Large‐Area MoS₂ on Graphene for High‐Responsivity Photodetectors

Controllable creating of wafer‐scale homogeneous vertical or parallel 2D heterostructures with low cost by the van der Waals stacking or covalently bonded stitching of 2D layered materials, such as graphene, hexagonal boron nitride, and transition‐metal dichalcogenides, is of great challenge. In this paper, a new green growth strategy for the fabrication of high‐quality large‐area and low‐cost vertical MoS₂/graphene heterostructures has been successfully demonstrated via electrochemical deposition in water solution, followed by an annealing process in chemical vapour deposition system for the first time. The vertical MoS₂/graphene heterostructures have been systematically investigated by the combined use of Raman spectroscopy, atomic force microscopy, X‐ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy. This simple, reliable, and environmentally friendly growth strategy on conducting monolayer graphene in a controlled manner opens up a new way for producing low‐cost, large‐area, and high‐quality vertical MoS₂/graphene heterostructures, which have promising applications not only in electronics and optoelectronics but also in the fields of catalysis and renewable energy.