Boosting photocatalytic hydrogen evolution enabled by SiO2-supporting chiral covalent organic frameworks with parallel stacking sequence

doi:10.1016/S1872-2067(24)60107-5

Abstract

Abstract:

Two-dimensional covalent organic frameworks (2D COFs) feature extended π-conjugation and ordered stacking sequence, showing great promise for high-performance photocatalysis. Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer, but the precise ordered alignment is limited due to the non-covalent π-stacking of COF layers, accordingly hindering out-of-plane transfer kinetics. Herein, we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO₂ microsphere. Compared to the achiral COF analogues, the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration, thereby affording superior photocatalytic performance in hydrogen evolution from water splitting. Taking the simplest ketoenamine-linked chiral COF as a shell of SiO₂ particle, the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g^-1 h^-1 along with the apparent quantum efficiency of 14.31% at 475 nm. Furthermore, the composite photocatalysts could be fabricated into a film device, displaying a remarkable photocatalytic performance of 178.0 mmol m^-2 h^-1 for hydrogen evolution. Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties.

Key words: Covalent organic framework, Photocatalysis, Hydrogen generation, Chiral induction, Core-shell structure

Zheng Lin, Wanting Xie, Mengjing Zhu, Changchun Wang, Jia Guo. Boosting photocatalytic hydrogen evolution enabled by SiO₂-supporting chiral covalent organic frameworks with parallel stacking sequence[J]. Chinese Journal of Catalysis, 2024, 64: 87-97.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60107-5

https://www.cjcatal.com/EN/Y2024/V64/I9/87

Figures/Tables 7

Scheme 1. (a) Preparation of SiO2@TpPa(Δ/Λ) via the chirality-induced amorphous-to-crystalline transformation route. (b) Illustration of layered AA-stacking of the chiral and achiral COF, respectively, reflecting the difference of interlayer charge transfer.

Fig. 1. (a) Circular dichroism spectra of the chiral/achiral microspheres. FT IR spectra (b) and PXRD pattern (c) of SiO2 and the composite microspheres. TEM images of SiO2 (d,e), achiral SiO2@TpPa-50 (f,g), SiO2@TpPa(Δ)-50 (h,i), and SiO2@TpPa(Λ)-50 (j,k).

Fig. 2. TEM images of SiO2@TpPa(Δ)-25 (a), SiO2@TpPa(Δ)-75 (b), and SiO2@TpPa(Δ)-90 (c). (d) Circular dichroism spectra of SiO2@TpPa (Δ) with different COF content.

Fig. 3. (a) UV-vis DRS. (b) Energy band structures of the photocatalysts. (c) Time course for photocatalytic H2 production under visible irradiation for SiO2 and SiO2@TpPa-50, SiO2@TpPa(Δ)-50, and SiO2@TpPa(Λ)-50. (d) Photocatalytic performances for a series of SiO2@TpPa(Δ)-X. (e) Comparison of the HER and AQE for SiO2@TpPa(Δ)-50 with the recently reported representative COF-based photocatalysts. (f) Comparison of the HER for the chiral TpPa photocatalysts synthesized using different methods.

Fig. 4. (a) Wavelength-dependent AQE of SiO2@TpPa(Δ)-50 superimposed with its absorption curve. (b) Recyclability of SiO2@TpPa(Δ)-50 for 10 cycles over 40 h under visible light irradiation. (c) HRTEM-EDS elemental mapping for the SiO2@TpPa(Δ)-50 after photocatalysis. (d) Photograph of the film device. (e) Photograph for the hydrogen gas produced from the film under irradiation. (f) Photocatalytic performance of the SiO2@TpPa(Δ)-50 film with different loading mass.

Fig. 5. (a) Electrochemical impedance spectra. (b) Transient photocurrent responses. (c) Time-resolved PL spectra. Time slices of the transient absorption spectra of SiO2@TpPa-50 (d) and SiO2@TpPa(Δ)-50 (e). (f) Femtosecond time-resolved transient absorption decay kinetics with fitting profiles. Surface potential images of SiO2@TpPa-50 (g) and SiO2@TpPa(Δ)-50 (h). (i) The calculated BEF of SiO2@TpPa-50 and SiO2@TpPa(Δ)-50.

Fig. 6. Top view of stacking structures and side view of the charge transport channels for the parallel-stacking TpPa-COF and antiparallel-stacking TpPa-COF. The calculated out-of-plane transfer rate kET are given at the bottom.

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Boosting photocatalytic hydrogen evolution enabled by SiO₂-supporting chiral covalent organic frameworks with parallel stacking sequence

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