Construction of highly active WO3/TpPa-1-COF S-scheme heterojunction toward photocatalytic H2 generation

doi:10.1016/j.jmst.2021.12.065

Abstract

Abstract:

The rapid charge recombination and low surface reaction kinetics are the two major constraints to the photocatalytic performance of covalent organic frameworks (COFs). To accelerate the charge separation behavior, TpPa-1-COF is decorated with WO₃ via an in-situ growth approach, and the resultant WO₃/TpPa-1-COF composites show significantly improved photocatalytic performance. Especially, when the WO₃ loading arrives at 3 wt%, 3%WO₃/TpPa-1-COF exhibits the maximum photocatalytic H₂ evolution rate of 19.89 mmol g^-1 h^-1, which is approximately 4.8 times higher than that of pure TpPa-1-COF. The apparent quantum efficiency (AQE) of 3%WO₃/TpPa-1-COF at 420 nm is detected to be 12.4%. X-ray photoelectron spectroscopy (XPS) characterization confirms the formation of internal electric field between WO₃ and TpPa-1-CF, which can drive the photogenerated charge carrier diffusion in S-scheme mode. As a result, WO₃/TpPa-1-COF composite possesses high charge separation efficiency and strong redox ability, which is further supported by the photoelectrochemical results, thus benefiting the photocatalysis process. This work provides a rational strategy to modify COFs in photocatalytic water splitting.

Key words: Covalent organic framework (COF), WO₃, S-scheme heterojunction, Photocatalytic H₂ evolution

Long Sun, Lingling Li, Jiajie Fan, Quanlong Xu, Dekun Ma. Construction of highly active WO₃/TpPa-1-COF S-scheme heterojunction toward photocatalytic H₂ generation[J]. J. Mater. Sci. Technol., 2022, 123: 41-48.

Figures/Tables 8

Fig. 1. (a) The systhesis process for WO3/TpPa-1-COF; (b-d) SEM images of TpPa-1-COF, pure WO3 and 3%WO3/TpPa-1-COF; (e, f) and TEM and HRTEM images of 3%WO3/TpPa-1-COF.

Fig. 2. (a, b) Small-angle and wide-angle XRD patterns and (c) FT-IR spectra of as-prepared samples. (d) N2 adsorption-desorption isotherms of TpPa-1-COF, WO3 and 3%WO3/TpPa-1-COF.

Table 1. Textural properities of synthesized samples.

Samples	S_BET (m²/g)	Average pore size (nm)	Pore volume (cm³/g)
TpPa-1-COF	925.9	2.7	0.64
3%WO₃/TpPa-1-COF	934.4	2.8	0.65
WO₃	5.6	35.6	0.05

Fig. 3. XPS survey spectra (a) and the high-resolution XPS spectra of C 1 s (b), N 1 s (c) and W 4f (d) of TpPa-1-COF, WO3 and 3%WO3/TpPa-1-COF.

Fig. 4. The UV-vis DRS spectra (a) and PL spectra with an excitation wavelength of 350 nm (b) of the synthesized samples; (c) TR-PL spectra with corresponding fitting results of TpPa-1-COF, WO3, and 3%WO3/TpPa-1-COF.

Fig. 5. (a) Comparison of the H2 evolution rate over the as-prepared samples and (b) stability evaluation of photocatalytic H2 evolution over 3%WO3/TpPa-1-COF under visible light irradiation (λ ≥ 420 nm).

Fig. 6. (a) Transient photocurrent response and (b) electrochemical impedance spectra of TpPa-1-COF, WO3 and 3%WO3/TpPa-1-COF; Mott-Schottky plots of TpPa-1-COF (c) and WO3 (d) at 2 kHz, 3 kHz and 4 kHz.

Fig. 7. Schematic type-II (a) and S-scheme (b) mechanism over WO3/TpPa-1-COF system; (c) TEM image of WO3/TpPa-1-COF after photo-deposition of Pt NPs, the inset: HRTEM of Pt NPs.

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Construction of highly active WO₃/TpPa-1-COF S-scheme heterojunction toward photocatalytic H₂ generation

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