Triazine-based COF/TiO2 S-scheme heterojunction with oxygen vacancies for efficient photocatalytic CO2 reduction

doi:10.1016/S1872-2067(26)64987-X

Abstract

Abstract:

Solar-driven CO₂ conversion into valuable hydrocarbon fuels process primarily depends on the development of efficient photocatalysts capable of achieving effective charge separation, high sunlight utilization, and strong reactant adsorption. In this work, one-dimensional (1D) TiO₂ nanobelts with abundant oxygen vacancies (TN) were strategically coupled with a two-dimensional (2D) electron-rich triazine-based covalent organic framework (CTF) to construct a high-efficiency 1D/2D TN/CTF S-scheme heterojunction for photocatalytic CO₂ reduction. The resulting TN/CTF composites exhibited impressive CO₂ conversion rates toward CO and CH₄ generation, with the optimized TN/CTF composite (TN/CTF10) achieving the highest CO and CH₄ yields of 21.4 and 7.9 μmol g^‒1 h^‒1, respectively, which were 3.5- and 4.4-fold higher than those of pristine CTF and represented 6.5- and 7.2-fold enhancements compared to pure TN. The charge-transfer mechanism involved in the S-scheme heterojunction was identified via photo-irradiated Kelvin probe force microscopy, in-situ X-ray photoelectron spectroscopy, and density functional theory calculations, while the formation of oxygen vacancies was confirmed by electron spin resonance and X-ray photoelectron spectroscopy. Further in-depth studies indicate that the oxygen vacancies in TN greatly broaden light absorption and provide an intermediate energy level that accelerates charge separation in the S-scheme heterojunction, thereby significantly improving light-harvesting efficiency and suppressing charge recombination. Meanwhile, the synergistic integration of defect engineering with S-scheme heterojunction design optimizes redox capability and CO₂ adsorption strength to enhance the CO₂ reduction reaction. This work offers a new perspective on designing high-performance photocatalysts by integrating defect engineering into S-scheme heterojunctions.

Key words: Photocatalysis, S-scheme heterojunction, Oxygen vacancy, CO₂ reduction

Keshan Tang, Wanyi Deng, Ningyuan Wang, Yang Xia, Xinhe Wu, Heng Yang. Triazine-based COF/TiO₂ S-scheme heterojunction with oxygen vacancies for efficient photocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2026, 83: 244-257.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)64987-X

https://www.cjcatal.com/EN/Y2026/V83/I4/244

Figures/Tables 9

Fig. 1. (a) Schematic synthesis process of the TN/CTF composite. (b) XRD patterns of P25, H2Ti2O5, TO and TN samples. (c) ESR spectra of pure TO, TN and TN/CTF10 samples.

Fig. 2. FESEM images of CTF (a) and TN/CTF10 (b) samples. TEM (c) and HRTEM (d) images of the TN/CTF10 composite. HAADF-STEM image (e) and the corresponding elemental mappings (f-i) of C, N, Ti, and O for the TN/CTF10 composite.

Fig. 3. XRD patterns of CTF and TN/CTF composites. (b) FT-IR spectra of CTF, TN, and TN/CTF10 samples (the light blue shaded region of the FT-IR spectra is magnified on the right). (c) N2 sorption-desorption isotherms. (d) Calculated isosteric heat (Qst) of CO2 adsorption on CTF, TN/CTF10, and TO/CTF10 samples.

Fig. 4. High-resolution XPS spectra of C 1s (a) and N 1s (b) for CTF and TN/CTF10 in the dark and under light irradiation. Ti 2p (c) and O 1s (d) for TN and TN/CTF10 in the dark and under light irradiation. CO2 adsorption on the TiO2 (101) plane based on DFT calculations in the absence of oxygen vacancies (e) and in the presence of oxygen vacancies (f). The red, brown, and light blue spheres represent O, C, and Ti atoms, respectively.

Fig. 5. (a) Control experiments for photocatalytic CO2 reduction over the TN/CTF10 sample under different reaction conditions. (b) photocatalytic CO2 reduction performance of the obtained samples under 300 W Xe lamp irradiation using saturated water vapor as the reductant. (c) cycling durability of photocatalytic CO2 reduction over TN/CTF10. (d) AQE values of the TN/CTF10 sample at different wavelengths.

Fig. 6. Steady-state PL emission spectra (a), TRPL spectra (b), transient photocurrent responses (c), and Nyquist plots of EIS spectra (d) for CTF, TO, TN, and TN/CTF10 samples.

Fig. 7. Surface morphology image of the TN/CTF10 composite (a) and corresponding surface potential maps in darkness (b) and under light irradiation (c). (d) Line-scanning surface potential from point A to point B.

Fig. 8. 2D transient absorption mapping, transient absorption spectra, and normalized decay kinetic curves for TN (a?c) and the TN/CTF10 composite (d?f).

Fig. 9. Calculated electrostatic potentials for the (001) facet of CTF (a) and the (101) facet of TN (b). (c) Proposed S-scheme charge transfer mechanism for the TN/CTF composite.

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Triazine-based COF/TiO₂ S-scheme heterojunction with oxygen vacancies for efficient photocatalytic CO₂ reduction

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