【摘要】 Photocatalytic hydrogen peroxide（H₂O₂） generation is largely subject to the sluggish conversion kinetics of the superoxide radical(O₂^.-) intermediate, which has relatively low reactivity and requires high energy.Here, we present a lattice-strain strategy to accelerate the conversion of O₂^.-to highly active singlet oxygen（¹O₂） by optimizing the distance between two adjacent active sites, thereby stimulating H₂O₂generation via low-barrier oxygen-oxygen coupling. As the initial demonstration, the defect-induced strain in Zn In₂S₄nanosheet optimizes the distance of two adjacent Zn sites from 3.85 to 3.56 ?, resulting in that Zn In₂S₄with 0.7% compressive strain affords 3086.00 μmol g^-1h^-1yield of H₂O₂with sacrificial agent.This performance is attributed to the strain-induced enhancement of electron coupling between the compressed adjacent Zn sites, which promotes low-barrier oxygen-oxygen coupling to active¹O₂intermediate. This finding paves the way for atomic-scale manipulation of reactive sites, offering a promising approach for efficient H₂O₂photosynthesis.更多还原

【Abstract】 Photocatalytic hydrogen peroxide（H₂O₂） generation is largely subject to the sluggish conversion kinetics of the superoxide radical(O₂^.-) intermediate, which has relatively low reactivity and requires high energy.Here, we present a lattice-strain strategy to accelerate the conversion of O₂^.-to highly active singlet oxygen（¹O₂） by optimizing the distance between two adjacent active sites, thereby stimulating H₂O₂generation via low-barrier oxygen-oxygen coupling. As the initial demonstration, the defect-induced strain in Zn In₂S₄nanosheet optimizes the distance of two adjacent Zn sites from 3.85 to 3.56 ?, resulting in that Zn In₂S₄with 0.7% compressive strain affords 3086.00 μmol g^-1h^-1yield of H₂O₂with sacrificial agent.This performance is attributed to the strain-induced enhancement of electron coupling between the compressed adjacent Zn sites, which promotes low-barrier oxygen-oxygen coupling to active¹O₂intermediate. This finding paves the way for atomic-scale manipulation of reactive sites, offering a promising approach for efficient H₂O₂photosynthesis.更多还原