Photo-thermal CO2 reduction with methane on group VIII metals: In situ reduced WO3 support for enhanced catalytic activity

doi:10.1016/S1872-2067(21)63835-4

Abstract

Abstract:

Photo-thermal CO₂ reduction with methane (CRM) is beneficial for solar energy harvesting and energy storage. The search for efficient photo-thermal catalysts is of great significance. Here, we reveal that group VIII metal catalysts supported by optical material WO₃ are more effective for photo-thermal CRM, giving catalytic activities with visible light assistance that are 1.4-2.4 times higher than that achieved under thermal conditions. The activity enhancement (1.4-2.4 times) was comparable to that achieved with plasmonic-Au-promoted catalysts (1.7 times). Characterization results indicated that WO₃ was partially reduced to WO_3-_x in situ under the reductive CRM reaction atmosphere, and that WO_3-_x rather than WO₃ enhanced the activities with visible light assistance. Our method provides a promising approach for improving the activity of catalysts under light irradiation.

Key words: Tungsten oxide, Visible light, In situ reduction, Photocatalysis, CO₂ reduction

Huimin Liu, Xianguang Meng, Weiwei Yang, Guixia Zhao, Dehua He, Jinhua Ye. Photo-thermal CO₂ reduction with methane on group VIII metals: In situ reduced WO₃ support for enhanced catalytic activity[J]. Chinese Journal of Catalysis, 2021, 42(11): 1976-1982.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63835-4

https://www.cjcatal.com/EN/Y2021/V42/I11/1976

Figures/Tables 6

Fig. 1. Catalytic performances of Rh/WO3 and Rh/TiO2 in CRM. (a) CO2 conversion; (b) CH4 conversion; (c) CO yield; (d) H2 yield. Reaction conditions: 500 °C, CH4/CO2 = 1, flow rate = 20.0 mL min-1, 0.050 g of catalyst, with or without visible light irradiation (500 nm < λ < 800 nm).

Fig. 2. XRD patterns (a), enlarged XRD patterns in the range of 32°-36° (b), UV-visible spectra (c), XPS spectra (d), and HRTEM images of Rh/WO3 (e) and Rh/TiO2 (f).

Table 1 Physicochemical properties of the supports and catalysts.

Catalyst	Rh loading^a (wt%)	A_BET^b (m² g^-1)
WO₃	—	5.1
Rh/WO₃	0.93	5.5
TiO₂	—	8.6
Rh/TiO₂	1.00	8.3

Fig. 3. (a) Wavelength ranges obtained with different filter sets; CH4 and CO2 conversions (b) and H2 and CO yields (c) obtained with Rh/WO3 without and with light irradiation with different wavelength ranges; (d) UV-visible spectra of fresh Rh/WO3 and spent Rh/WO3 (400-1000 nm) and AE/photon. Reaction conditions: 500 °C, CH4/CO2 = 1, flow rate = 20.0 mL min-1, 0.050 g of catalyst.

Fig. 4. (a) W 4f XPS spectra of Rh/WO3 and spent Rh/WO3, with the blue and orange lines denoting the peaks of W6+ and W5+, respectively; (b) H2-TPR profiles of WO3 and Rh/WO3; XRD pattern (c) and UV-visible spectrum (d) of spent Rh/WO3.

Fig. 5. In situ ESR profiles of fresh and spent Rh/WO3 in CO2 atmosphere with and without visible light irradiation.

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Photo-thermal CO₂ reduction with methane on group VIII metals: In situ reduced WO₃ support for enhanced catalytic activity

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