Selective CO2 photoreduction to CH4 mediated by dimension-matched 2D/2D Bi3NbO7/g-C3N4 S-scheme heterojunction

doi:10.1016/S1872-2067(21)63819-6

Abstract

Abstract:

Discovering highly selective catalysts is key to achieve effective CO₂photoreduction to hydrocarbon fuels. In this work, we construct an ultrathin dimension-matched S-scheme Bi₃NbO₇/g-C₃N₄ heterostructure, which permits the highly selective photocatalytic reduction of CO₂ to CH₄, as shown by ¹³C isotopic measurements. Density functional theory calculations combined with solid-state characterization confirm the electron transfer from g-C₃N₄ nanosheets to Bi₃NbO₇, establishing an internal electric field. The internal electric field drives photogenerated electrons from Bi₃NbO₇ to g-C₃N₄, as revealed by in-situ X-ray photoelectron spectroscopy, demonstrating the presence of an S-scheme charge transfer path in Bi₃NbO₇/g-C₃N₄ heterostructures allowing efficient and selective CO₂ photoreduction. As a result, the optimized sample achieved a CH₄ evolution rate of 37.59 μmol·g ^-1·h ^-1, a ca. 15-fold enhancement compared to ultrathin g-C₃N₄ nanosheets, and also retained stability after 10 reaction cycles and 40 h of simulated solar irradiation with no sacrificial reagents. The optimized Bi₃NbO₇/g-C₃N₄ composites achieve almost 90% selectivity for CH₄ production over CO.

Key words: Dimension-matched, S-scheme, Photocatalysis, CO₂ reduction, Selectivity

Kai Wang, Xuezhen Feng, Yangzi Shangguan, Xiaoyong Wu, Hong Chen. Selective CO₂ photoreduction to CH₄ mediated by dimension-matched 2D/2D Bi₃NbO₇/g-C₃N₄ S-scheme heterojunction[J]. Chinese Journal of Catalysis, 2022, 43(2): 246-254.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63819-6

https://www.cjcatal.com/EN/Y2022/V43/I2/246

Figures/Tables 8

Fig. 1. (a) Schematic illustration of the preparation of dimension-matched hybrid photocatalyst BNO/UCN (Bi3NbO7/g-C3N4); (b) TG curves of UCN and BNO/UCN-X (X = 1, 2, 3, 4); (c) FTIR spectra of the samples.

Fig. 2. (a) AFM image and height cutaway view of BNO/UCN-3; HRTEM image (b), HAADF-STEM image and EDX elemental mapping images (c) of BNO/UCN-3.

Fig. 3. Comparison of Bi 4f (a), Nb 3d (b), C 1s (c), and N 1s (d) XPS spectra for BNO, UCN, and BNO/UCN-3 in the dark or under light irradiation.

Fig. 4. (a) UV-VIS DRS spectra of selected samples; TRPL (b), SPV (c) spectra, and transient photocurrent (d) of selected samples.

Fig. 5. Electrostatic potentials of the Bi3NbO7 (200) (a) and C3N4 (001) (b) surfaces along the Z-axis; Charge density difference (c) and ELF (d) of the BNO/UCN interface.

Fig. 6. ESR signals of DMPO-•O2? (a) and DMPO-•OH (b) for different samples; (c) Schematic illustration of S-scheme charge transfer paths at the BNO/UCN interface. DMPO: dimethylpyrroline-N-oxide.

Fig. 7. (a) CO2 adsorption isotherms of BNO, UCN, and BNO/UCN-3; (b) Photocatalytic CO2 reduction to CO, and CH4 (c); (d) Products of CO2 photoreduction using BNO (red), UCN (blue), and BNO/UCN-3 (orange) catalysts; (e) Cycling experiments for CO2 photoreduction by BNO/UCN-3; (f) GC-MS spectra of products formed by BNO/UCN-3 with 12C- (top) and 13C-labeled (bottom) CO2.

Fig. 8. In-situ FTIR spectra of BNO/UCN-3 and reaction pathway of photochemical CO2 conversion on BNO/UCN.

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Selective CO₂ photoreduction to CH₄ mediated by dimension-matched 2D/2D Bi₃NbO₇/g-C₃N₄ S-scheme heterojunction

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