Stabilizing F-Al-O active center via confinement of Al2O3 in SiC framework for conversion of 1,1-difluoroethane greenhouse gas

JOURNAL OF FLUORINE CHEMISTRY(2024)

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摘要
Al2O3 exhibits high activity for the resource utilization of potent greenhouse gases, hydrofluorocarbons via dehydrofluorination or F/Cl exchange. However, it experiences completely fluorination under corrosive HF environment, leading to thorough fluorination of F-Al-O active site into F-Al-F, accompanied with serious carbon deposition. In this work, we successfully confined Al2O3 in SiC (Al2O3@SiC) via treating Al2O3/SiC under high temperatures (>800 degrees C). The results showed that different with simple loaded Al2O3(Al2O3/SiC), during high temperature treatment, reaction between Al2O3 and SiC occurred, leading to the confinement effect. Then, contributed by the interaction, desired F-Al-O species could be stabilized on the surface of SiC. While for Al2O3/SiC, it thoroughly turned into AlF3 under identical reactive conditions, leading to inferior stability during CH3CHF2 dehydrofluorination. Furthermore, the reaction rate of 5 %Al2O3@SiC is nearly up to 4 folds higher than that of traditional AlF3. Facilitated by the suitable Lewis acid intensity, less carbon deposition formed on Al2O3@SiC. Thus, constructing strong interaction between F-Al-O and stable SiC provides a potential strategy to stabilize unstable active centers.
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关键词
SiC,Dehydrofluoriantion,Greenhouse gases,Hydrofluorocarbons,F-Al-O
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