Thiadiazole-functionalized covalent triazine frameworks for constructing S-scheme heterojunctions enabling boosted H2O2 photosynthesis

doi:10.1016/S1872-2067(26)65079-6

Abstract

Abstract:

Photocatalytic hydrogen peroxide (H₂O₂) generation from water and air provides a prospective means for converting solar energy into valuable chemicals, which, however, is limited by the low carrier separation efficiency of traditional single-component semiconductor photocatalysts. Herein, we report a facile strategy for constructing an S-scheme organic heterojunction by integrating graphitic carbon nitride (g-C₃N₄) with covalent triazine frameworks (CTFs). The thiadiazole-modified CTFs are precisely functionalized with benzothiadiazole, phenyl, and biphenyl groups. The hybrid with optimized structure achieves a 3259 μmol g⁻¹ h⁻¹ H₂O₂ generation rate, outperforming pristine CTFs and g-C₃N₄ by 78-fold and 8-fold, respectively. In-situ characterizations confirm the enhanced light absorption, redox capacity, and charge carrier dynamics of the g-C₃N₄/CTF S-scheme heterojunction. The thiadiazole units increase active sites within CTFs and collaborate with g-C₃N₄ to accelerate electron-hole separation and enable high H₂O₂ selectivity. Through theoretical/experimental analyses, the O₂ adsorption configuration on CTFs is revealed to favor a two-step single-electron O₂ reduction route, reducing thermodynamic barriers for O₂-to-H₂O₂ conversion. Providing design strategies for organic heterojunctions with enhanced electronic structures, this study enables efficient artificial H₂O₂ photosynthesis.

Key words: C₃N₄, Covalent triazine frameworks, S-scheme heterojunction, Thiadiazole active sites, Photosynthesis of H₂O₂

Gaoxiong Liu, Rundong Chen, Bingquan Xia, Xianlong Zhou, Laiquan Li, Shantang Liu. Thiadiazole-functionalized covalent triazine frameworks for constructing S-scheme heterojunctions enabling boosted H₂O₂ photosynthesis[J]. Chinese Journal of Catalysis, 2026, 87: 170-184.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65079-6

https://www.cjcatal.com/EN/Y2026/V87/I8/170

Figures/Tables 7

Fig. 1. Scheme depicting the H2O2 production via photo-redox reactions on the COF-based heterojunction photocatalyst.

Fig. 2. (a) Illustration of routes for synthesizing CN/CTF samples. (b) XRD patterns of CN/CTF composites. (c) FT‐IR spectra of CN, CTF and CNC-TD-X composites. TEM image (d) and magnified TEM image (e) of CNC-TD-10. HAADF-STEM image of CNC-TD-10 (f) and corresponding elemental distribution for C (g), N (h), and S (i).

Fig. 3. (a) UV-DRS spectra of CN, CTF-TD and the CNC-TD-10 composites. (b) Corresponding Tauc plots derived from the Kubelka-Munk function. Mott-Schottky plots of CN (c) and CTF-TD (d). (e) Proposed diagram illustrating the S-scheme band alignment between CN and CTF-TD. PL spectra (f) and TRPL spectra (g) for CN, CTF-TD and CNC-TD-10. Photocurrent responses (h) and EIS Nyquist plots (i) for CNC-TD-10, CNC-CB-10 and CNC-BP-10.

Fig. 4. XPS spectra and photocatalytic activities (a) S 2p spectra for CTF-TD and CNC-TD-10. C 1s (b) and N 1s (c) spectra for CNC-TD-10 and CN. Surface morphology and corresponding KPFM images of CN (d), CNC-TD-10 (e), and CTF-TD (f). Surface potential scanning curves of CN (g), CNC-TD-10 (h), and CTF-TD (i) under dark and illuminated conditions.

Fig. 5. (a) H2O2 production performance of CTF-based photocatalysts under varying gas atmospheres (λ ≥ 420 nm, 300 W Xe lamp, 100 mW cm−2; 10 mg catalyst, 25 mL ethanol aqueous solution (10 vol%)). (b) Performance comparison of different CTFs (CTF-TD, CTF-CB, and CTF-BP) and corresponding CN/CTF hybrids for photocatalytic H2O2 production. (c) H2O2 production performance over CN, CTF-TD, and CN/CTF-TD- hybrids under 60 min of simulated irradiation. (d) Recycle tests of CNC-TD-10 for H2O2 production.

Fig. 6. (a) EPR spectra of DMPO-•O2− signals for CN, CTF-TD, and CNC-TD-10 measured in MeOH under O2 saturation and light exposure. EPR spectra of TEMP-1O2 signals (b) and DMPO-•OH signals (c) for CN, CTF-TD, and CNC-TD-10 measured in aqueous suspension. In-situ DRIFTS spectra tracking intermediates during H2O2 photosynthesis over CNC-TD-10 (d), CNC-CB-10 (e), and CNC-BP-10 (f). (g) The energies of O2 adsorption at the S and N sites on the CTF backbone in both pristine CTF and the CTF segment within cyanide-modified conjugated triazine frameworks with thiadiazole units (CNC-TD) systems. DFT?calculated Gibbs free energy diagrams for the •O2− (h) and 1O2 (i) transformation pathways during the O2-to-H2O2 conversion over CNC-TD.

Fig. 7. (a) Proposed mechanism of S-scheme charge transfer in CN/CTF-TD (Ef denotes the Fermi level). (b) Schematic diagram of charge transfer and active sites in the S-scheme heterojunction. (c) Schematic illustration of the proposed mechanism for H2O2 synthesis via the ORR pathway on the S-scheme heterojunction.

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Thiadiazole-functionalized covalent triazine frameworks for constructing S-scheme heterojunctions enabling boosted H₂O₂ photosynthesis

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