Graphene Quantum Dots‐Decorated 2D CuInP2S6 Nanosheets with Specially Enhanced Heterojunction‐Associated Photocatalytic Activity for High‐Performance Water Decontamination

The significant environmental challenges of dye‐contaminated wastewater necessitate efficient photocatalyst for pollutant degradation. Herein, a novel graphene quantum dots (GQDs) modified CuInP 2 S 6 composite (GQDs@CuInP 2 S 6 ) with a type‐II band alignment has been successfully synthesized via laser liquid phase melting technology. Under visible light, GQDs@CuInP 2 S 6 achieves 98.3% degradation of Rhodamine B (RhB) within 8 min, exhibiting a kinetic rate constant 2–3 orders of magnitude higher than pristine CuInP 2 S 6 . Density functional theory calculations reveal this enhancement stems from unique electronic modulation of CuInP 2 S 6 by GQDs. Notably, irrespective of van der Waals or covalent GQDs‐CuInP 2 S 6 interactions, the composite transitions from pristine CuInP 2 S 6 's a indirect bandgap to a direct bandgap, with chemisorbed GQDs further narrowing the gap, which facilitates electron transition and broadens light absorption spectrum. Additionally, the band alignment and partial charge density confirm a type‐II heterojunction in chemisorbed GQDs@CuInP 2 S 6 . Holes from GQDs@CuInP 2 S 6 and electrons from CuInP 2 S 6 generate an internal electric field, suppressing charge carrier recombination and significantly enhancing photocatalytic performance. This work pioneers a synthesis approach for quantum dot‐decorated surface composite and theoretically elucidates the quantum dot modification mechanisms, advancing a new innovative photocatalytic material design.