Solar-energy-driven photothermal catalytic C-C coupling from CO2 reduction over WO3-x

doi:10.1016/S1872-2067(21)63868-8

Abstract

Abstract:

Solar-energy-driven catalytic CO₂ reduction for the production of value-added carbon-based materials and chemical raw materials has attracted great interest to alleviate the global climate change and energy crisis. The production of multicarbon (C2) products through CO₂ reduction is extremely attractive, however, the yield and selectivity of C2 products remain low because of the low reaction temperature required and the low photoelectron density of the substrate. Here, we introduce WO_3-_x, which contains oxygen vacancies and exhibits an excellent photothermal conversion efficiency, to improve the generation of C2 products (C₂H₄ and C₂H₆) under simulated sunlight (UV-Vis-IR) irradiation. WO_3-_x produced 5.30 and 0.93 μmol·g^-1 C₂H₄ and C₂H₆, respectively, after 4 h, with a selectivity exceeding 34%. In situ Fourier transform infrared spectra and theoretical calculations showed that the oxygen vacancies enhanced the water activation and hydrogenation of adsorbed CO for the formation of C2 products via C-C coupling from CH₂/CH₃ intermediates. The findings of this study could assist in the design of highly active solar-energy-driven catalysts to produce C-C coupling products through CO₂ reduction.

Key words: WO₃, Oxygen vacancy, CO₂ reduction, Photothermal, C-C coupling

Yu Deng, Jue Li, Rumeng Zhang, Chunqiu Han, Yi Chen, Ying Zhou, Wei Liu, Po Keung Wong, Liqun Ye. Solar-energy-driven photothermal catalytic C-C coupling from CO₂ reduction over WO_3-_x[J]. Chinese Journal of Catalysis, 2022, 43(5): 1230-1237.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63868-8

https://www.cjcatal.com/EN/Y2022/V43/I5/1230

Figures/Tables 5

Fig. 1. The characterization results of different samples. (a) XRD patterns of WO3 and WO3?x; (b) HRTEM images of WO3?x; (c) Intensity profiles along the arrows in b and the corresponding elemental mapping of W and O of WO3?x; (d) ESR spectra; (e) O 1s XPS spectra; (f) Raman spectra of WO3 and WO3?x.

Fig. 2. (a) UV-Vis-IR DRS spectra of WO3 and WO3-x. (b) Temperature-time variation curve under UV-Vis-IR irradiation; Photothermal images after 5 min of UV-Vis-IR irradiation: blank (c), WO3 (d), and WO3-x (e).

Fig. 3. Light-induced catalytic performance of WO3 and WO3-x; (a) CO, (b) CH4, (c) C2H4, and (d) C2H6 generation; (e) Comparison between the hydrocarbon fuel production rates over WO3-x under UV-Vis, IR, and UV-Vis-IR irradiation, and 73, 106, and 177 °C; (f) On-line gas chromatography mass spectrum of the WO3-x catalyzed CO2 reduction under UV-Vis-IR light irradiation.

Fig. 4. CO2 adsorption (a) and TPD (b) of WO3 and WO3-x; Photocurrent responses (c), electrochemical impedance spectra (d), PL spectra (e), and time-resolved PL spectra (f) of WO3 and WO3-x.

Fig. 5. In-situ FTIR spectra indicating the adsorption and activation of CO2 in the presence of H2O on WO3-x between 1000 and 1800 cm-1 (a) and 2900 and 3400 cm-1 (b). Differential charge density diagrams (0.04 electrons/Å3) of C1 adsorbed on the material surface: (c) CO2 adsorbed on WO3, (d) CO adsorbed on WO3, (e) CO2 adsorbed on WO3-x, and (f) CO adsorbed on WO3-x. Differential charge density diagrams (0.003 electrons/Å3) of C2 adsorbed on the material surface: (g) CH3 + CH3 adsorbed on WO3, (h) CH2 + CH2 adsorbed on WO3, (i) CH3 + CH3 adsorbed on WO3-x, (j) and CH2 + CH2 adsorbed on WO3-x.

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Solar-energy-driven photothermal catalytic C-C coupling from CO₂ reduction over WO_3-_x

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