Interfacial engineering of a plasmonic Ag/Ag2CO3/C3N5 S-scheme heterojunction for high-performance photocatalytic degradation of antibiotics

doi:10.1016/S1872-2067(25)64652-3

Abstract

Abstract:

Devising S-scheme heterostructure is considered as a cutting-edge strategy for advanced photocatalysts with effectively segregated photo-carriers and prominent redox potential for emerging organic pollutants control. Herein, an S-scheme Ag₂CO₃/C₃N₅ heterojunction photocatalyst was developed via a simple in situ chemical deposition procedure, and further photoreduction operation made metallic Ag (size: 3.5-12.5 nm) being in situ formed on Ag₂CO₃/C₃N₅ for a plasmonic S-scheme Ag/Ag₂CO₃/C₃N₅ heterojunction photocatalyst. Consequently, Ag/Ag₂CO₃/C₃N₅ manifests pronouncedly upgraded photocatalytic performance toward oxytetracycline degradation with a superior photoreaction rate constant of 0.0475 min^‒1, which is 13.2, 3.9 and 2.2 folds that of C₃N₅, Ag₂CO₃, and Ag₂CO₃/C₃N₅, respectively. As evidenced by comprehensive characterizations and density functional theory calculations, the localized surface plasmon resonance effect of metallic Ag and the unique S-scheme charge transfer mechanism in 0D/0D/2D Ag/Ag₂CO₃/C₃N₅ collaboratively strengthen the visible-light absorption, and facilitate the effective separation of powerful charge carriers, thereby significantly promoting the generation of reactive species like ·OH^-, h⁺ and ·O₂^- for efficient oxytetracycline destruction. Moreover, four consecutive cycles demonstrate the reusability of Ag/Ag₂CO₃/C₃N₅. Furthermore, the authentic water purification tests affirm its practical application potential. This work not only provides a candidate strategy for advancing S-scheme heterojunction photocatalysts but also makes a certain contribution to water decontamination.

Key words: Localized surface plasmon resonance, S-scheme, Ag/Ag₂CO₃/C₃N₅, Antibiotic removal, Internal electric field

Shijie Li, Xinyu Li, Yanping Liu, Peng Zhang, Junlei Zhang, Bin Zhang. Interfacial engineering of a plasmonic Ag/Ag₂CO₃/C₃N₅ S-scheme heterojunction for high-performance photocatalytic degradation of antibiotics[J]. Chinese Journal of Catalysis, 2025, 72: 130-142.

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Figures/Tables 7

Fig. 1. (a) Schematic synthesis process of Ag/Ag2CO3/C3N5. TEM images of C3N5 (b) and Ag/Ag2CO3/C3N5-2 (c). (d) The size distribution of Ag/Ag2CO3 NPs. HRTEM image (e) and EDS mapping (f) of Ag/Ag2CO3/C3N5-2.

Fig. 2. (a) XRD characterization. XPS profiles of C3N5, Ag2CO3, and Ag/Ag2CO3/C3N5-2: whole spectra (b), Ag 3d (c), N 1s (d), C 1s (e), and O 1s (f).

Fig. 3. Photocatalytic LEV (a) and OTC destruction outcomes (c) and kinetic rate constants (b,d) over C3N5, Ag2CO3, Ag2CO3/C3N5, Ag/Ag2CO3/C3N5-1, Ag/Ag2CO3/C3N5-2, and Ag/Ag2CO3/C3N5-3 catalysts. (e) The catalytic efficacy of Ag/Ag2CO3/C3N5-2 in the presence of HA. (f) The catalytic performance of Ag/Ag2CO3/C3N5-2 in the presence of various anions. (g) The treatment efficacy of Ag/Ag2CO3/C3N5-2 in authentic waters. (h) Cyclic catalytic performance of Ag/Ag2CO3/C3N5-2. (i) Effects of various scavengers on photocatalytic LEV eradication over Ag/Ag2CO3/C3N5-2.

Fig. 4. (a) Decomposition course of OTC over Ag/Ag2CO3/C3N5-2. (b-d) Eco-toxicity appraisal.

Fig. 5. (a) UV-vis DRS of as-fabricated samples. the corresponding Kubeka-Munk profiles (b,c), Mott-Schottky curves (d,e), and UPS spectra (f) of C3N5 and Ag2CO3. (g) S-scheme charge redistribution mechanism.

Fig. 6. In-situ irradiated XPS analyses for Ag 3d (a), O 1s (b), and N 1s (c) of Ag/Ag2CO3/C3N5-2. Calculated Φ values of Ag2CO3 (d) and C3N5 (e). Calculated 3D (f) and 2D (g) charge density difference distribution. Transient photocurrent response spectra (h) and EIS (i) of C3N5, Ag2CO3, Ag2CO3/C3N5 and Ag/Ag2CO3/C3N5-2.

Fig. 7. (a) Adsorption energies of O2 and H2O molecules on different sites of Ag/Ag2CO3/C3N5-2. (b,c) EPR detection of ?O2- and ?OH signals over Ag/Ag2CO3/C3N5-2. (d) Proposed mechanism of photocatalytic antibiotic destruction in the Ag/Ag2CO3/C3N5-2 system.

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Interfacial engineering of a plasmonic Ag/Ag₂CO₃/C₃N₅ S-scheme heterojunction for high-performance photocatalytic degradation of antibiotics

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