The efficient utilization of solar energy is the actual task of the present and near future. Thus, the preparation of appropriate materials that are able to harvest and utilize the broad wavelength range of solar light (especially commonly ignored near-infrared light region-NIR) is the high-priority challenging mission. Our study provides a rationally designed two-dimensional (2D) flexible heterostructures with photocatalytic activity for the production of "clean" hydrogen under NIR illumination, with the hydrogen production rate exceeding most 2D materials and the ability to use the seawater as a starting material. The proposed design utilizes the hybrid bimetallic (Au/Pt) periodic structure, which is further covalently grafted with a metal-organic framework MIL-101(Cr). The periodic gold structure is able to efficiently support the plasmon-polariton wave and to excite the hot electrons, which is further injected in the Pt and MIL-101(Cr) layers. The Pt and MIL-101(Cr) structures provide catalytic sites, which are saturated with hot electrons and efficiently initiate water splitting and hydrogen production. The MIL-101(Cr) layer also serves for repelling generated hydrogen bubbles. The mechanistic studies reveal the catalytic role of every element of the 2D flexible heterostructures. The maximum hydrogen output was achieved under plasmon resonance excitation in the NIR range, and it could be actively controlled by the applied LED wavelength.
Keywords: metal−organic frameworks; near-infrared light; plasmon catalysis; water splitting.