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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]
Xiaoli Wei, Yiwei Sun, Jianhai Jiang, Zhen Wang, Wei Zhang, Bing Liu, Shucheng Wang, Xiaodan Yang, Wanjin Yu, Jianjun Zhang, Wenfeng Han
ABSTRACT

Al 2 O 3 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 Al 2 O 3 in SiC (Al 2 O 3 @SiC) via treating Al 2 O 3 /SiC under high temperatures (>800 °C). The results showed that different with simple loaded Al 2 O 3 (Al 2 O 3 /SiC), during high temperature treatment, reaction between Al 2 O 3 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 Al 2 O 3 /SiC, it thoroughly turned into AlF 3 under identical reactive conditions, leading to inferior stability during CH 3 CHF 2 dehydrofluorination. Furthermore, the reaction rate of 5 %Al 2 O 3 @SiC is nearly up to 4 folds higher than that of traditional AlF 3 . Facilitated by the suitable Lewis acid intensity, less carbon deposition formed on Al 2 O 3 @SiC. Thus, constructing strong interaction between F-Al-O and stable SiC provides a potential strategy to stabilize unstable active centers.

MATERIALS

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