All-organic covalent organic frameworks/perylene diimide urea polymer S-scheme photocatalyst for boosted H2 generation

doi:10.1016/S1872-2067(22)64130-5

Abstract

Abstract:

Conjugated covalent organic frameworks (COFs) hold great promise in photocatalytic hydrogen evolution owing to their high crystallinity, large surface area, and distinct structure. However, COFs exhibit poor charge separation. Therefore, investigating highly effective COF-based photocatalysts is crucial. For the first time, conjugated COF/perylene diimide urea polymer (PUP) all-organic heterostructure with S-scheme interfacial charge-transfer channels was successfully developed and manufactured via in situ coupling of the two-dimensional triazine-based imine-linked COF (denoted as TATF-COF) with PUP. The optimal photocatalytic hydrogen-evolution rate of 94.5 mmol h^-1 g^-1 for TATF-COF/PUP is 3.5 times that of pure TATF-COF and is comparable to or even higher than that of the previously reported COF-based photocatalysts, resulting in an apparent quantum efficiency of up to 19.7% at 420 nm. The improved directional S-scheme charge transfer driven by the tuned built-in electric field and enhanced oxidation and reduction reaction rates of the photogenerated carriers contribute synergistically to the boosted photocatalytic H₂ evolution. Experiments and theoretical studies reveal plausible H₂ evolution and spatial S-scheme charge-separation mechanisms under visible-light irradiation. This study provides advanced methods for constructing all-organic S-scheme high-efficiency photocatalysts by the modulation of band structures.

Key words: Covalent organic framework, Photocatalytic hydrogen evolution, S-Scheme heterostructure, Perylene diimide urea polymer, Spatial charge-separation mechanism

Zizhan Liang, Rongchen Shen, Peng Zhang, Youji Li, Neng Li, Xin Li. All-organic covalent organic frameworks/perylene diimide urea polymer S-scheme photocatalyst for boosted H₂ generation[J]. Chinese Journal of Catalysis, 2022, 43(10): 2581-2591.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64130-5

https://www.cjcatal.com/EN/Y2022/V43/I10/2581

Figures/Tables 8

Fig. 1. Schematic of synthesizing the TATF-COF/PUP sample.

Fig. 2. (a) Experimental diffraction patterns (black), patterns simulated from the structural model (blue), and profiles calculated from residual (green) and Le Bail fitting (pink) for TATF-COF. (b) XRD patterns for TATF-COF, PUP, and TATF-COF/PUP. (c) Solid-state 13C NMR spectra of TATF-COF, PUP, and TATF-COF/PUP and the signal assignments (inset). (d) AA stacking model of top and side views of TATF-COF. (e) FTIR spectra for TATF-COF, PUP AND TATF-COF/PUP.

Fig. 3. (a) TEM, (b) and (c) SEM images of TATF-COF/PUP, and (d) energy dispersive X-ray spectra of TATF-COF/PUP corresponding to the elemental mapping of C, O, and N (e?g).

Fig. 4. (a) Average hydrogen-evolution rates over the TATF-COF, PUP, and TATF-COF/PUP composites. (b) Photocatalytic stability of the TATF-COF/PUP photocatalyst. (c) Wavelength dependence of AQE. (d) AQE of TATF-COF/PUP-3 mg compared with that of recently reported COF-based catalysts.

Fig. 5. (a) SPV spectra. TPV spectra of the (b) TATF-COF and (c) TATF-COF/PUP composites. (d) Time-resolved fluorescence decay spectra of the TATF-COF, PUP, and TATF-COF/PUP composites. (e) Steady-state PL spectra. (f) Transient photocurrent response.

Fig. 6. (a) UV-Vis diffuse-reflectance spectra and optical images (inset). XPS valence band spectra of (b) TATF-COF and (c) PUP. M-S plots of redox potentials (d) of TATF-COF and (e) PUP. (f) Schematic of the bandgaps of TATF-COF and PUP.

Fig. 7. Molecular orbital distribution of the (a) HOMO and (b) LUMO. (c) Work function of TATF-COF. Molecular orbital distribution of the (d) HOMO and (e) LUMO. (f) Work function of PUP.

Fig. 8. (a) UPS spectra of TATF-COF and PUP. (b) ESR spectra under the visible-light illumination. (c) Proposed mechanism of S-scheme heterojunction for TATF-COF/PUP.

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All-organic covalent organic frameworks/perylene diimide urea polymer S-scheme photocatalyst for boosted H₂ generation

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