Interface Engineering of MoS 2 -Modified Graphitic Carbon Nitride Nano-photocatalysts for an Efficient Hydrogen Evolution Reaction.

Understanding of photochemical charge transfer processes at nanoscale heterojunctions is essential in developing effective catalysts. Here, we utilize a controllable synthesis method and a combination of optical absorption, photoluminescence, and electrochemical impedance spectroscopic studies to investigate the effect of MoS ₂ nanosheet lateral dimension and edge length size on the photochemical behavior of MoS ₂ -modified graphitic carbon nitride (g-C ₃ N ₄ ) heterojunctions. These nano-heterostructures, which comprise interlayer junctions with variable area (i. e., MoS ₂ lateral size ranges from 18 nm to 52 nm), provide a size-tunable interfacial charge transfer through the MoS ₂ /g-C ₃ N ₄ contacts, while exposing a large fraction of surface MoS ₂ edge sites available for the hydrogen evolution reaction. Importantly, modification of g-C ₃ N ₄ with MoS ₂ layers of 39±5 nm lateral size (20 wt % loading) creates interfacial contacts with relatively large number of MoS ₂ edge sites and efficient electronic transport phenomena, yielding a high photocatalytic H ₂ -production activity of 1497 μmol h ^-1 g _cat ^-1 and an apparent QY of 3.3 % at 410 nm light irradiation. This study thus offers a design strategy to improve light energy conversion efficiency of catalysts by engineering interfaces at the nanoscale in 2D-layered heterojunction materials.
(© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)