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Improving Charge Carrier Separation through S-Scheme-Based 2D–2D WS<sub>2</sub>/Sulfur-Doped g-C<sub>3</sub>N<sub>4</sub> Heterojunctions for a Superior Photocatalytic O<sub>2</sub> Reduction Reaction

Kundan Kumar Das, Upali Aparajita Mohanty, Ritik Mohanty, Preeti Prabha Sarangi, Dipti Prava Sahoo, Kulamani Parida

2024ACS Applied Energy Materials40 citationsDOI

Abstract

Hydrogen peroxide (H 2 O 2 ) generation via a photocatalytic O 2 reduction reaction has been considered an economically efficient and environmentally friendly synthesis method. However, the productivity of H 2 O 2 production is restricted because of sluggish reaction kinetics and fast recombination of photoinduced excitons. Therefore, a superior two-dimensional (2D)–2D WS 2 /sulfur-doped g-C 3 N 4 (WSCN) hybrid material was successfully fabricated to address the associated limitations through a combination of wet impregnation and calcination techniques for H 2 O 2 production. The effective anchoring of WS 2 nanoplates onto sulfur-doped g-C 3 N 4 (SCN) nanosheets facilitates effective separation of photoinduced excitons with sturdy redox properties, which is attributable to the establishment of S-scheme heterojunctions between WS 2 and SCN through W–S bonding as substantiated by X-ray photoelectron spectroscopy (XPS) analysis. The W–S bond at the interface acts as a bridge for effective charge segregation pathways. Among all, 2.5 WSCN displays an exceptional H 2 O 2 production of 817 μmol, which was 7.9- and 2.68-fold higher than those of pristine WS 2 and SCN, respectively. The solar-to-chemical conversion efficiency was found to be 0.24%, whereas the apparent quantum yield was estimated to be 3.19% at 420 nm irradiation. The improved photocatalytic activity was figured out by a higher cathodic photocurrent of −1.51 mA cm –2 and delayed recombination of excitons, as supported by photoluminescence and electrochemical impedance spectroscopy measurements. The S-scheme charge-transfer pathway was well validated by a radical scavenging experiment and work function, which was evaluated from VB-XPS analysis and in situ XPS measurement. This research offers a paradigmatic idea for constructing an S-scheme photocatalyst for H 2 O 2 generation.

Topics & Concepts

X-ray photoelectron spectroscopyHeterojunctionMaterials sciencePhotocurrentDielectric spectroscopyPhotocatalysisPhotoluminescencePhotoinduced charge separationExcitonDopingCharge carrierCalcinationPhotochemistryElectrochemistryChemical engineeringOptoelectronicsChemistryCatalysisPhysical chemistryArtificial photosynthesisElectrodeOrganic chemistryPhysicsEngineeringQuantum mechanicsAdvanced Photocatalysis TechniquesGas Sensing Nanomaterials and SensorsPerovskite Materials and Applications