Naphthalenediimide-Based Polymer Dots with Dual Acceptors as a New Class of Photocatalysts for Photocatalytic Hydrogen Generation under Visible Light Irradiation

Organic-conjugated polymer dots (Pdots) are emerging as promising photocatalysts for solar-driven hydrogen production. However, organic solvents are commonly used as cosolvents in photocatalytic systems to promote the dispersion of organic materials and improve the overall efficiency of the photocatalytic process. Herein, two naphthalenediimide (NDI)-based Pdots, with and without surfactant, are fabricated and presented as highly efficient and stable photocatalysts for visible-light-driven hydrogen generation in a solvent-free organic system for the first time. The prepared Pdots exhibit high photocatalytic activity and remarkable photostability. Achieving high efficiency and long-term photostability is essential for the future commercialization of large-scale hydrogen production. Furthermore, the NDI-BTF-PS-PEG-COOH Pdots of the dual acceptor (A₁-D-A₂-D system) consisting of a strong acceptor (NDI, A₁) and a weak acceptor (BTF, A₂) exhibit high photocatalytic efficiencies and stabilities with Pt-cocatalyst over 72 h. Thus, constructing A₁-D-A₂-D NDI-based Pdots is a promising approach to developing efficient and stable photocatalysts for solar-driven hydrogen production.