Photo-enhanced thermal catalytic CO2 methanation activity and stability over oxygen-deficient Ru/TiO2 with exposed TiO2 {001} facets: Adjusting photogenerated electron behaviors by metal-support interactions

doi:10.1016/S1872-2067(21)63825-1

Abstract

Abstract:

In this study, two Ru/TiO₂ samples with different TiO₂ facets were prepared to investigate their photo-thermal catalytic CO₂ + H₂ reaction behavior. Without UV irradiation, the Ru/TiO₂ with 67% {001} facet (3RT) displayed improved thermal catalytic activity for CO₂ methanation than that of Ru/TiO₂ with 30% {001} facet (0RT). After H₂ pretreatment, both samples exhibited enhanced thermal catalytic activities, but the H₂-treated 3RT (3RT-H) exhibited superior activity to that of the H₂-treated 0RT (0RT-H). Under UV irradiation, 3RT-H exhibited apparent photo-promoted thermal catalytic activity and stability, but the enhanced catalytic activity was lower than that of 0RT-H. Based on the characterization results, it is proposed that both the surface oxygen vacancies (Vos) (activating CO₂) and the metallic Ru nanoparticles (activating H₂) were mainly responsible for CO₂ methanation. For 0RT, H₂ pretreatment and subsequent UV irradiation did not promote the formation of Vos, resulting in low catalytic activity. For 3RT, on the one hand, H₂ pretreatment promoted the formation of Vos, which were regenerated under UV irradiation; on the other hand, the photogenerated electrons from TiO₂ transferred to Ru to maintain the metallic Ru nanoparticles. Both behaviors promoted the activation of CO₂ and H₂ and enhanced CO₂ methanation. Moreover, the photogenerated holes favored the dissociated H at Ru migrating to TiO₂, also promoting CO₂ methanation. These behaviors occurring on 3RT-H may be attributed to the suitable metal-support interaction between the Ru nanoparticles and TiO₂ {001}, resulting in the easy activation of lattice oxygen in TiO₂to Vos. With reference to the analysis of intermediates, a photo-thermal reaction mechanism is proposed for the Ru/TiO₂ {001} facet sample.

Key words: Photo-thermal CO₂ reduction, Oxygen vacancy, Ru/TiO₂, Metal-support interaction

Ke Wang, Shihui He, Yunzhi Lin, Xun Chen, Wenxin Dai, Xianzhi Fu. Photo-enhanced thermal catalytic CO₂ methanation activity and stability over oxygen-deficient Ru/TiO₂ with exposed TiO₂ {001} facets: Adjusting photogenerated electron behaviors by metal-support interactions[J]. Chinese Journal of Catalysis, 2022, 43(2): 391-402.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63825-1

https://www.cjcatal.com/EN/Y2022/V43/I2/391

Figures/Tables 9

Fig. 1. XRD patterns (a) and UV-vis DRS spectra (b) of 0T, 3T, 0RT, and 3RT; SEM images of 0RT (c) and 3RT (d), and TEM images of 0RT (e) and 3RT (f).

Fig. 2. TPR profiles (a), XPS spectra (b) of the Ru species; EPR (c) and XPS (d) spectra of the O species within the various samples.

Fig. 3. CO2 methanation using 0RT (a), 3RT (b), 0RT-H (c), and 3RT-H (d); (e) Stability of 3RT-H at 300 °C under UV irradiation or in darkness; (f) Action spectrum of 3RT-H at 300 °C.

Fig. 4. XPS spectra, after various treatments, of Ru and C species on 0RT-H (a) and 3RT-H (b). (1) After H2 treatment; (2) After CO2 methanation without UV irradiation, (3) After CO2 methanation under UV irradiation. The quasi-situ electron paramagnetic resonance spectra, after various treatments, of 0RT-H (c) and 3RT-H (d).

Fig. 5. In situ DRIFS spectra of CO2 activation at various temperatures on 0RT-H (a) and 3RT-H (c) in darkness, and 0RT-H (b) and 3RT-H (d) under UV irradiation.

Fig. 6. In situ DRIFS spectra of CO2 + H2 methanation at various temperatures on 0RT-H (a) and 3RT-H (c) in darkness, and 0RT-H (b) and 3RT-H (d) under UV irradiation.

Fig. 7. H2-pulse studies of 0RT-H (a) and 3RT-H (c) in darkness, and 0RT-H (b) and 3RT-H (d) under UV irradiation.

Fig. 8. (a) Photocurrent (inset: electrochemical impedance spectra), (b) PL spectra, and (c) Fluorescence emission decay spectra of various samples; (d) Charge carrier transfer mechanism on 3RT-H.

Fig. 9. Possible mechanisms of CO2 methanation over 3RT-H with or without ultraviolet (UV) irradiation. Upper: the thermal CO2 methanation, bottom: the photo-thermal CO2 methanation.

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Photo-enhanced thermal catalytic CO₂ methanation activity and stability over oxygen-deficient Ru/TiO₂ with exposed TiO₂ {001} facets: Adjusting photogenerated electron behaviors by metal-support interactions

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