LAUSR

Abstract Transferable 2-dimensional (2D) MoS2 thin films have a versatile potential for constructing highly efficient photoelectrodes when combined with conventional semiconductor light absorbers, taking advantage of its optical transparency and high electrochemical activity. Here, we firstly report fully vertically aligned MoS2 (VMS)/p-Si heterostructure photocathode for photoelectrochemical (PEC) water splitting. Furthermore, 3D iron-nickel sulfide nanoparticles of tailored atomic composition are formed simultaneously during the synthesis of VMS via one-step sulfurization to build 3D/2D transition metal sulfide (TMD) heterostructure thin film catalyst. The spectroscopic results reveal that the Fe-doped Ni3S2 nanoparticles on VMS/p-Si photocathode induce the electrochemically-benign band bending in the overall heterostructure, enabling a significant improvement in PEC performance and long-term stability. Scanning photoelectrochemical microscopy is used to vividly visualize the photocurrent enhancement by the various 3D/2D TMD heterostructures. This work provides promising strategies in developing high performance TMD-based electrocatalysts for practical applications in a wide variety of electrochemical energy conversion processes.