Na2CO3-assisted synthesis of Na-doped crystalline/amorphous g-C3N4 S-scheme homojunction photocatalyst for enhanced H2O2 production

doi:10.1016/S1872-2067(25)64849-2

Abstract

Abstract:

The construction of crystalline/amorphous g-C₃N₄ homojunctions presents a versatile strategy to obtain all-organic homojunction photocatalysts with better interface matching and lower interface charge carrier movement resistance for optimized photocatalytic activity. However, the process entails a complex multi-step workup, which compromises its feasibility. To overcome this challenge, this work provided an innovative Na₂CO₃-induced crystallinity modulation strategy to construct a Na-doped crystalline/amorphous g-C₃N₄ S-scheme homojunction photocatalyst in a single step. The approach involves the initial pre-assembling of melamine and cyanuric acid molecules, and subsequent introduction of Na₂CO₃ before the calcination. Na₂CO₃ plays key roles to induce in-situ crystallinity modulation during the calcination and as a source for Na-doping. The prepared g-C₃N₄ S-scheme homojunction photocatalyst demonstrated a prominent H₂O₂-production rate of 444.6 μmol·L^-1·h^-1, which is 6.1-fold higher than that of bulk g-C₃N₄. The enhanced activity was attributed to the synergistic effect of charge carrier separation induced by the S-scheme homojunction system, and the optimized interfacial H₂O₂generation kinetics. The latter was fostered by the Na-doping. This study provides an innovative approach for the one-step construction of g-C₃N₄ S-scheme homojunction and its integration in photocatalytic applications.

Key words: Photocatalysis, S-scheme homojunction, Crystalline/amorphous g-C₃N₄, Crystallinity modulation, H₂O₂ production

Lihong Tan, Xinhe Wu, Jiachao Xu, Mahmoud Sayed, Guohong Wang. Na₂CO₃-assisted synthesis of Na-doped crystalline/amorphous g-C₃N₄ S-scheme homojunction photocatalyst for enhanced H₂O₂ production[J]. Chinese Journal of Catalysis, 2025, 79: 174-185.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64849-2

https://www.cjcatal.com/EN/Y2025/V79/I12/174

Figures/Tables 6

Fig. 1. (A) Graphical illustration for synthesizing amorphous g-C3N4 and Na-doped crystalline/amorphous g-C3N4 homojunction. (B) Synthesis mechanism diagram of crystalline g-C3N4. (C) XRD patterns of precursors. (D) Magnified XPS spectra in the 850?1300 eV range of the different precursors.

Fig. 2. XRD patterns (A), the typical (002) diffraction peaks (B), XPS survey spectra (C), high-resolution XPS spectra of Na 1s (D), O 1s (E), N 1s (F), locally magnified images of N 1s (G), C 1s (H), and FT-IR spectra (I) of samples.

Fig. 3. SEM images of BCN (A), CN (B), and Na0.5-CCN/CN (C) samples. TEM images (D1?D3), HRTEM images (D4), and EDX elemental mapping images (E?H) of Na0.5-CCN/CN.

Fig. 4. (A) UV-vis diffused reflectance spectra. (B) Tauc plots. (C) Band alignments. The calculated density of state (DOS) and electrostatic potential of C3N4 (D,F) and Cyano-C3N4 (E,G). Energy band o?sets (H) and interfacial charge transfer (I) in C3N4/Cyano-C3N4 homojunction.

Fig. 5. (A,B) Photocatalytic H2O2-production activities. (C) Time-dependent curves of photocatalytic decomposition of H2O2. (D) Photocatalytic cycling test. (E,F) Performance comparison of different samples. (G) Schematic illustration of photocatalytic H2O2-generation mechanism.

Fig. 6. (A,B) Optimized models. (C) O2 adsorption energy. (D) COHP analyses of *OOH adsorption on C3N4 and Na-C3N4. (E) Gibbs free energy of *OOH radical. Transient photocurrent responses (F), EIS curves (G), and steady-state (H) and transient-state (I) PL spectra of samples.

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Na₂CO₃-assisted synthesis of Na-doped crystalline/amorphous g-C₃N₄ S-scheme homojunction photocatalyst for enhanced H₂O₂ production

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