“Environmental phosphorylation” boosting photocatalytic CO2 reduction over polymeric carbon nitride grown on carbon paper at air-liquid-solid joint interfaces

doi:10.1016/S1872-2067(21)63824-X

Abstract

Abstract:

The limited CO₂ content in aqueous solution and low adsorption amount of CO₂ on catalyst surface lead to poor photocatalytic CO₂ reduction activity and selectivity. Herein, the design and fabrication of a novel photocatalytic architecture is reported, accomplished via chemical vapor deposition of polymeric carbon nitride on carbon paper. The as-obtained samples with a hydrophobic surface exhibit excellent CO₂ transport and adsorption ability, as well as the building of triphase air-liquid-solid (CO₂-H₂O-catalyst) joint interfaces, eventually resulting in the inhibition of H₂evolution and great promotion of CO₂ reduction with a selectivity of 78.6%. The addition of phosphate to reaction environment makes further improvement of CO₂ photoreduction into carbon fuels with a selectivity of 93.8% and an apparent quantum yield of 0.4%. This work provides new insight for constructing efficient photocatalytic architecture of CO₂ photoreduction in aqueous solution and demonstrates that phosphate could play a key role in this process.

Key words: Photocatalytic CO₂ reduction, Hydrophobic surface, Air-liquid-solid triphase interfaces, Mass transport, Phosphorylation

Qinghe Zhang, Yang Xia, Shaowen Cao. “Environmental phosphorylation” boosting photocatalytic CO₂ reduction over polymeric carbon nitride grown on carbon paper at air-liquid-solid joint interfaces[J]. Chinese Journal of Catalysis, 2021, 42(10): 1667-1676.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63824-X

https://www.cjcatal.com/EN/Y2021/V42/I10/1667

Figures/Tables 7

Fig. 1. Scheme of the triphase photocatalytic architecture and mechanism of the triphase photocatalysis.

Fig. 2. (a) FESEM image of LCP and the corresponding water contact angle (inset of a); (b) FESEM image of CN/LCP and the corresponding water contact angle (inset of b); (c) The enlarged FESEM image of CN grown on LCP; (d) FESEM image of BCP and the corresponding water contact angle (inset of d); (e) FESEM image of CN/BCP and the corr esponding water contact angle (inset of e); (f) The enlarged FESEM image of CN grown on BCP.

Fig. 3. CO2 adsorption isotherms (a) and UV-vis DRS (b) of various samples; (c) UV-vis DRS of the scraped samples; (d) Steady-state PL spectra of various samples.

Fig. 4. Powder XRD patterns (a) and FTIR spectra (b) of various samples; High-resolution XPS spectra of C 1s (c) and N 1s (d) of CN/LCP.

Fig. 5. (a) Photocatalytic CO2 reduction property of CN/LCP and CN/BCP in pure water in the triphase photocatalytic system; (b) Photocatalytic CO2 reduction property of CN/LCP and CN/BCP completely immersed in pure water; (c-e) Schematic illustration of the diphase and triphase photocatalytic systems.

Fig. 6. (a) GC-MS analysis of CO labeled by 13C and 12C from CRR over CN/LCP in pure water; (b) Cycling test of photocatalytic activity over CN/LCP in pure water

Fig. 7. (a) Photocatalytic property of CN/LCP in Na3PO4 (0.1 M) solution; (b) Photocatalytic activity in NaCl (0.1 M) solution and pH-adjusted NaCl solution (0.1 M, pH = 12).

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“Environmental phosphorylation” boosting photocatalytic CO₂ reduction over polymeric carbon nitride grown on carbon paper at air-liquid-solid joint interfaces

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