Synergistic Ag single atoms and nanoclusters on defect-engineered In2S3 for enhanced H2O2 production and in-situ pollutant oxidation

Nitrogen doping introduces sulfur vacancies and lattice distortion into In 2 S 3 , which enhances charge separation and provides anchoring sites for Ag species. • Achieves a high H 2 O 2 production rate of 965 μmol g −1 ·h −1 via the 2e − ORR pathway. • DFT reveals Ag single atoms optimize *OOH adsorption; clusters boost electron redistribution. • Exhibits efficient degradation of perphenazine (95% removal within 30 min). • Operates effectively in pure water without sacrificial agents and shows excellent stability. To address the rapid recombination of photogenerated charge carriers in indium sulfide (In 2 S 3 ) and meet the growing demand for efficient photocatalytic hydrogen peroxide (H 2 O 2 ) production systems, this study proposes a rational design. Leveraging active nitrogen species generated from urea decomposition during hydrothermal treatment, we successfully doped the In 2 S 3 lattice to construct a nitrogen-modified indium sulfide (N-In 2 S 3 ) substrate, and subsequently co-anchored silver single atoms and clusters (Ag SA+C /N-In 2 S 3 ) onto it for efficient photocatalytic H 2 O 2 production and pollutant degradation. Nitrogen (N) doping induced sulfur vacancies and lattice distortion, enhancing charge separation and surface reactivity. Ag species were atomically dispersed and firmly anchored onto the N-In 2 S 3 support, serving as efficient electron sinks and active sites. The optimized Ag SA+C /N-In 2 S 3 achieved a remarkable H 2 O 2 production rate of 965 μmol g −1  h −1 in pure water via a predominant two-electron oxygen reduction reaction (2e − ORR) pathway, significantly outperforming pristine In 2 S 3 and N-In 2 S 3 . Combined with experimental characterization and DFT calculations revealed that Ag single atoms optimized the adsorption of the *OOH intermediate and reduced the reaction free energy barrier, while Ag clusters facilitated electron redistribution and enhanced oxygen activation. It also demonstrated superior photocatalytic degradation efficiency for organic pollutant like perphenazine (95% removal in 30 min). This study highlights the synergistic effect of bulk doping and surface atomic-level engineering in developing high-performance photocatalysts for sustainable chemical synthesis and environmental remediation. Download: Download high-res image (140KB) Download: Download full-size image