doi:10.1016/S1872-2067(22)64143-3

Abstract

Abstract:

Constructed by selecting appropriate building blocks, covalent organic frameworks (COFs) can be endowed with a variety of specific functions. Herein, we successfully synthesized an imine-linked H₂PReBpy-COF with the CO₂ reduction catalyst [Re^I(bpy)(CO)₃Cl] and the porphyrin photosensitizer as the monomeric building units. The light-harvesting properties of the porphyrin itself, augmented by the extended π-conjugated planar structure of 2D COF, enable H₂PReBpy-COF the excellent light-harvesting capability, efficient charge separation, and fast interfacial charge transfer. In addition, a large amount of uniformly distributed [Re^I(bpy)(CO)₃Cl] units offer H₂PReBpy-COF an excellent activity toward photocatalytic CO₂ reduction with moderate selectivity and reusability. This study demonstrated a proof of concept in which the advantages of COFs and functional monomers are rationally integrated for photocatalytic solar fuel conversion.

Key words: Covalent organic framework, CO₂ photoreduction, Porphyrin, Re complex, Visible-light

Dengmeng Song, Wenhua Xu, Jun Li, Jiale Zhao, Qing Shi, Fei Li, Xuzhuo Sun, Ning Wang. "All-in-one" covalent organic framework for photocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2022, 43(9): 2425-2433.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64143-3

https://www.cjcatal.com/EN/Y2022/V43/I9/2425

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Fig. 1. (a) Schematic showing the synthesis of H2PReBpy-COF. (b) PXRD patterns of experimental H2PReBpy-COF (blue) and simulated for AA stacking (yellow). (c) The ideal AA eclipsed structures for H2PReBpy-COF from the views of top.

Fig. 2. (a) XPS survey of H2PReBpy-COF and H2PBpy-COF. (b) Re 4f XPS spectrum of H2PReBpy-COF. (c) and (d) BET surface areas (inset illustration: pore size distribution diagram) of H2PReBpy-COF and H2PBpy-COF.

Fig. 3. SEM (a) and HR-TEM (b) images, and the elemental mapping (c) of H2PReBpy-COF.

Fig. 4. UV-vis DRS (a) and the corresponding Tauc plots (b) of H2PReBpy-COF and H2PBpy-COF. (c) LUMO and HOMO positions of H2PReBpy-COF and H2PBpy-COF. (d) Transient photocurrent signals for H2PReBpy-COF and H2PBpy-COF. (e) EIS Nyquist plots of H2PReBpy-COF and H2PBpy-COF. (f) Time-resolved PL decay profiles of H2PReBpy-COF and H2PBpy-COF.

Fig. 5. (a) CO and HCOOH produced during the CO2 photoreduction on H2PReBpy-COF. (b) Catalysis performance under various reaction conditions. (c) The mass spectrum for the gas product and (d) the 13C NMR spectra for the liquid product in the photocatalytic reduction of 13CO2.

Fig. 6. (a) PET route of H2PReBpy-COF under light excitation. (b) The proposed photocatalytic mechanism of H2PReBpy-COF.

Fig. 7. Schematic of the calculated energy profile for the elementary steps during CO2 reduction process by simplified models.

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"All-in-one" covalent organic framework for photocatalytic CO₂ reduction

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"All-in-one" covalent organic framework for photocatalytic CO2 reduction

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"All-in-one" covalent organic framework for photocatalytic CO₂ reduction