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

作　　者：Weilu Wang Xiangke Zeng Yanliu Dang Ping Ouyang Haidong Zhang Guangming Jiang Fan Dong Tao Yang Steven L.Suib Yang He 

机构地区：[1]Engineering Research Center for Waste Oil Recovery Technology and Equipment,Ministry of Education,Chongqing Technology and Business University,Chongqing 400067,China [2]Institute of Materials Science,University of Connecticut,Storrs,CT 06269,United States [3]Yangtze Delta Region Institute(Huzhou)&Institute of Fundamental and Frontier Sciences,University of Electronic Science and Technology of China,Huzhou 313001,China [4]College of Chemistry and Chemical Engineering,Chongqing University,Chongqing 401331,China [5]Department of Chemical,Biological and Materials Engineering,University of South Florida,Tampa,FL 33620,United States

出　　处：《Chinese Chemical Letters》2022年第3期1346-1352,共7页中国化学快报（英文版）

基　　金：financially supported by the Scientific and Technological Research Program of Chongqing Municipal Education Commission (Nos. KJQN202000823 and KJZD-K201900802);Research project of Chongqing Technology and Business University(No. 1956058);Scientific Platform Project;Ministry of Education (No. fykf201905);US Department of Energy Office of Basic Energy Sciences,Division of Chemical,Biological and Geological Sciences (No. DE-FG02-86ER13622.A000) for support of this research。

摘　　要：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 

分 类 号：TQ426[化学工程]