Pt single atoms/g-C3N4 photocatalysts enabling simultaneous H2 production and CO2 absorption through formic acid photoreforming

Abstract

Single-atom catalysts (SACs) have emerged as a frontier in heterogeneous catalysis due to their maximum metal atom utilization and unique electronic properties, offering promising pathways for efficient hydrogen production. Here, we report a robust strategy for synthesizing platinum (Pt) single atoms onto graphitic carbon nitride (g-C₃N₄) supports via strong coordination interactions. The stable, Pt single atoms enable full utilization of active sites and the selective dehydrogenation pathway for high performance formic acid (FA) oxidation. The resulting catalysts exhibit excellent photocatalytic performance for FA oxidation, achieving a total hydrogen yield of 55.8 mmol g⁻¹ h⁻¹ and 5.2 mol g_Pt⁻¹ h⁻¹ under acidic conditions (pH = 2.2). Moreover, under alkaline conditions (pH = 12.2), the catalyst drives a unique, clean, and selective FA oxidation process with negligible CO₂ emissions, but at the expense of significantly lower H₂ production rates. This work not only demonstrates a scalable approach for engineering densely populated SACs but also establishes a new benchmark for simultaneous H₂ production and CO₂ absorption via light-driven FA oxidation. The strategy provides a promising foundation for the development of next-generation SACs for green energy applications.