Highly efficient UV-visible-infrared photothermocatalytic removal of ethyl acetate over a nanocomposite of CeO2 and Ce-doped manganese oxide

doi:10.1016/S1872-2067(21)63816-0

Abstract

Abstract:

A unique nanocomposite of CeO₂nanoparticles and Ce-doped manganese oxide nanofibers having a crystalline cryptomelane-type octahedral molecular sieve (KMn₈O₁₆·nH₂O, abbreviated as OMS-2) structure (denoted CeO₂-CeOMS-2) was prepared by the reaction of Ce(NO₃)₃and KMnO₄ at 90 °C. CeO₂-CeOMS-2 shows extremely high photothermocatalytic activity, very low selectivity for acetaldehyde (an unfavorable byproduct), and excellent durability for ethyl acetate removal under UV-visible-infrared (UV-vis-IR) irradiation. In striking contrast, pure CeO₂, pure OMS-2, and TiO₂ (P25) showed much lower photothermocatalytic activities and higher selectivities for acetaldehyde. The CO₂ production rate within the first five minutes (r_CO2) of reaction with CeO₂-CeOMS-2 was as high as 1102.5 μmol g ^-1 min ^-1, which is 137, 17, and 30-times higher than those of pure CeO₂, pure OMS-2, and TiO₂ (P25), respectively. CeO₂-CeOMS-2 also shows good photothermocatalytic activity under vis-IR (λ > 420 or 560 nm) irradiation. Further, even under vis-IR (λ > 830 nm) irradiation, efficient photothermocatalytic activity was achieved. In addition, the catalytic activity of CeO₂-CeOMS-2 is far superior to those of pure CeO₂ and OMS-2, which is attributed to the fact that Ce doping significantly improves the lattice oxygen activity of OMS-2. The high photothermocatalytic activity of CeO₂-CeOMS-2 arises from the synergy between the photocatalytic effect of the CeO₂ nanoparticles and light-driven thermocatalysis of the Ce-doped OMS-2. The novel photoactivation of Ce-doped OMS-2, which is unlike that of conventional photocatalysis on semiconductor photocatalysts, further promotes the catalytic activity because the surface oxygen activity of Ce-doped OMS-2 is promoted upon UV-vis-IR or vis-IR (λ > 560 nm) irradiation.

Key words: Photocatalysis, Photothermocatalytis, Volatile orgamic compound, Ethylacetate oxidation, Manganese oxides

Long Zhang, Yi Yang, Yuanzhi Li, Jichun Wu, Shaowen Wu, Xin Tan, Qianqian Hu. Highly efficient UV-visible-infrared photothermocatalytic removal of ethyl acetate over a nanocomposite of CeO₂and Ce-doped manganese oxide[J]. Chinese Journal of Catalysis, 2022, 43(2): 379-390.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63816-0

https://www.cjcatal.com/EN/Y2022/V43/I2/379

Figures/Tables 11

Fig. 1. XRD patterns of CeO2-CeOMS-2 (1), OMS-2 (2), and CeO2 (3).

Fig. 2. TEM image (a), high-resolution (HR)TEM image of nanoparticle (b), and nanofiber (c) of CeO2-CeOMS-2.

Fig. 3. Mn 2p (a), Mn 3s (b), and Ce 3d (c) XPS spectra of CeO2-CeOMS-2.

Fig. 4. Ethyl acetate conversion (a) and acetaldehyde selectivity (b) with time, and initial CO2 production rate (c) of the catalysts under UV-vis-IR irradiation; Long-term photothermocatalytic ethyl acetate oxidation over CeO2-CeOMS-2 under UV-vis-IR irradiation (d).

Fig. 5. Ethyl acetate conversion (a) and acetaldehyde selectivity (b) with time, and CO2 production rate (c) of CeO2-CeOMS-2 under vis-IR and IR irradiation.

Fig. 6. (a) Optical absorption spectra of the catalysts; (b) Photocatalytic activity of CeO2-CeOMS-2 for ethyl acetate oxidation under UV-vis-IR irradiation at near room temperature; The equilibrium temperature (Teq) values of the catalysts under UV-vis-IR irradiation (c) and CeO2-CeOMS-2 under vis-IR and IR irradiation (d).

Fig. 7. Ethyl acetate conversion (a), acetaldehyde selectivity (b), and CO2 yield (c) of the catalysts for thermocatalytic oxidation of ethyl acetate at different temperatures in the dark.

Fig. 8. FTIR spectra obtained during the course of ethyl acetate oxidation over CeO2-CeOMS-2 at 200 °C in the presence of 18O2 (a) and that measured in the presence of 16O2 at 200 °C over the used CeO2-CeOMS-2 sample obtained after the 18O2 isotope experiment (b). Note: The peak corresponding to C16O2 around 2341 cm-1 is overlapped with that of C16O18O at around 2343 cm-1.

Fig. 9. CO-TPR profiles (a) and Raman spectra (b) of CeO2-CeOMS-2, OMS-2, and CeO2.

Fig. 10. Ethyl acetate reaction rates for catalytic ethyl acetate oxidation on CeO2-CeOMS-2 at different temperatures (a) and temperature-programmed reduction of CeO2-CeOMS-2 in the presence of ethyl acetate and the absence of O2 (b) in the dark and under the irradiation of UV-vis-IR and vis-IR (λ > 560 nm).

Scheme 1. Schematic of the synergy between photocatalysis on nano-CeO2, light-driven thermocatalysis on CeO2-CeOMS-2, and photoactivation.

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Highly efficient UV-visible-infrared photothermocatalytic removal of ethyl acetate over a nanocomposite of CeO₂and Ce-doped manganese oxide

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