1. FeO–CeO2 nanocomposites: an efficient and highly selective catalyst system for photothermal CO2 reduction to CO.
- Author
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Zhao, Jiaqing, Yang, Qi, Shi, Run, Waterhouse, Geoffrey I. N., Zhang, Xin, Wu, Li-Zhu, Tung, Chen-Ho, and Zhang, Tierui
- Subjects
CATALYST selectivity ,CARBON monoxide ,FISCHER-Tropsch process ,METHANE as fuel ,FOURIER transform infrared spectroscopy ,METHANOL ,PHOTOTHERMAL conversion ,CARBON dioxide ,CATALYSTS - Abstract
Solar-driven catalysis is a promising strategy for transforming CO
2 into fuels and valuable chemical feedstocks, with current research focusing primarily on increasing CO2 conversion efficiency and product selectivity. Herein, a series of FeO–CeO2 nanocomposite catalysts were successfully prepared by H2 reduction of Fe(OH)3 -Ce(OH)3 precursors at temperatures (x) ranging from 200 to 600 °C (the obtained catalysts are denoted as FeCe-x). An FeCe-300 catalyst with an Fe:Ce molar ratio of 2:1 demonstrated outstanding performance for photothermal CO2 conversion to CO in the presence of H2 under Xe lamp irradiation (CO2 conversion, 43.63%; CO selectivity, 99.87%; CO production rate, 19.61 mmol h−1 gcat −1 ; stable operation over 50 h). Characterization studies using powder X-ray diffraction and high-resolution transmission electron microscopy determined that the active catalyst comprises FeO and CeO2 nanoparticles. The selectivity to CO of the FeCe-x catalysts decreased as the reduction temperature (x) increased in the range of 300–500 °C due to the appearance of metallic Fe0 , which introduced an additional reaction pathway for the production of CH4 . In situ diffuse reflectance infrared Fourier transform spectroscopy identified formate, bicarbonate and methanol as important reaction intermediates during light-driven CO2 hydrogenation over the FeCe-x catalysts, providing key mechanistic information needed to explain the product distributions of CO2 hydrogenation on the different catalysts. Catalysis: Reclaiming carbon dioxide A nanomaterial that helps convert carbon dioxide to more useful chemicals has been developed by researchers in China. One potential method is to convert the carbon dioxide into carbon monoxide using a reaction known as reverse water-gas shift, and then use further reactions to convert this into fuel, or produce useful chemicals such as methanol or methane. This reaction normally requires high temperatures, and a catalyst is required to make the conversion efficient at lower, more practical temperatures. Tierui Zhang from the Technical Institute of Physics and Chemistry in Beijing and co-workers developed a nanocomposite based on iron and cerium with excellent performance in converting carbon dioxide into carbon monoxide with hydrogen only under light irradiation. This result indicates the potential of solar-driven catalysis for transforming carbon dioxide into fuels. A series of FeO-CeO2 nanocomposite catalysts (FeCe-x) were successfully fabricated by hydrogen reduction of hydroxide precursors at temperatures (x) between 200–600 °C. A FeCe-300 catalyst with a Fe:Ce ratio of 2-1 exhibited excellent performance for photothermal CO2 hydrogenation to CO (CO selectivity = 99.87%, CO production rate 19.61 mmol h−1 gcat −1 , excellent stability). The FeO phase was effective in promoting the reverse water-gas shift (RWGS, CO2 + H2 → CO + H2 O). Catalysts prepared at higher reduction temperatures contained both Fe0 and FeO, with the Fe0 catalyzing the Sabatier reaction (CO2 + 4H2 → CH4 + 2H2 O) and thus lowering FeCe-x catalyst selectivity to CO. [ABSTRACT FROM AUTHOR]- Published
- 2020
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