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Fe doped aluminoborate PKU-1 catalysts for the ketalization of glycerol to solketal: Unveiling the effects of iron composition and boron

引用

Chinese Chemical Letters 2022年第3期33卷 1346-1352页

作者： Weilu Wang Xiangke Zeng Yanliu Dang Ping Ouyang Haidong Zhang Guangming Jiang Fan Dong Tao Yang Steven L.Suib Yang He Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of EducationChongqing Technology and Business UniversityChongqing 400067China Institute of Materials Science University of ConnecticutStorrsCT 06269United States Yangtze Delta Region Institute(Huzhou)&Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaHuzhou 313001China College of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China Department of Chemical Biological and Materials EngineeringUniversity of South FloridaTampaFL 33620United States

An inexpensive Fe doped aluminoborate consisted of 18% Fe in PKU-1 material that exhibits high selectivity of 4-hydroxymethy-2,2-dimethyl^(-1),3-dioxolane (Solketal, 98.3%), considerable activity (TOF 51.7 h-1), and recyclable ability in the ketalization of glycerol to Solketal with acetone at 318 K has been developed. Our study demonstrated that the structure of Fe (less agglomerated iron species vs. FeO clusters) can be tuned by changing Fe loading in the PKU-1 material, which correlated well with experimental observations. Furthermore, the surface boron sites were promoted by iron loading and behaved as Lewis-acid sites to facilitate the reaction process of glycerol ketalization, while the Solketal selectivity was closely related with the structure of iron species in PKU-1, which was proved by kinetic studies, density function theory (DFT) calculations, and a series of spectroscopy studies. This investigation demonstrates that the surface B sites can play important roles in the reaction instead of being spectators.

关键词： Fe doping aluminoborate Glycerol recycling Ketalization boron reaction sites Lewis-acid dominating catalyst

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