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Fluorinated Mg–Al Hydrotalcites Derived Basic Catalysts for Transesterification of Glycerol with Dimethyl Carbonate

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Abstract

A series of fluorinated Mg–Al hydrotalcite-like (HTl) compounds were prepared by introduction of different amount of (AlF6)3− into HTl sheets via co-precipitation method. The fluorine-modified Mg–Al mixed oxides (CHT-F) with mesoporous structure were then acquired by thermal decomposition of as-prepared HTl precursors. The influence of fluorine modifier on the physicochemical properties of CHT-F samples was studied in detail and the results demonstrated that their structure and basicity were strongly related to the fluorine content. Simultaneously, the CHT-F samples were test for the glycerol carbonate (GC) production via transesterification between glycerol and dimethyl carbonate without organic solvent. For these catalysts, the role of basic sites was examined based on reactant conversion and product selectivities in overall reaction as well as in side reaction identified in this work. The catalytic results showed that the activity of CHT-F catalysts depended on the total number of surface basic sites. However, further study demonstrated that the undesired product was catalyzed by strong basic sites, resulting in decrease of GC selectivity. Thus, the introduction of appropriate amount of (AlF6)3− into the HTl structure can promote the production of GC, and the best catalytic performance was obtained over the catalyst with F:Al = 1.0. Besides, various parameters including reaction time, reaction temperature and catalyst amount were investigated to optimize the reaction conditions. Furthermore, these CHT-F catalysts possessed high stability on the basis of reusability test and catalyst characterization.

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Acknowledgements

Authors acknowledge the financial support from “Strategic Priority Research Program-Climate Change: Carbon Budget and Related Issues” of the Chinese Academy of Sciences Grants (XDA05010108), National Natural Science Foundation of China (21401164), the Natural Science Foundation of Shandong Province, China (ZR2016BL21, ZR2013BL019), and National Training Programs of Innovation and Entrepreneurship for Undergraduates (311190805, 311190806, 201510904007).

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Authors and Affiliations

  1. College of Chemistry, Chemical Engineering and Materials Science, Zaozhuang University, Zaozhuang, 277160, China

    Xuelan Zhang, Dengfeng Wang & Jie Ma

  2. CAS Key Lab of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, China

    Xuelan Zhang & Wei Wei

Authors
  1. Xuelan Zhang
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  2. Dengfeng Wang
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  3. Jie Ma
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  4. Wei Wei
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Correspondence to Xuelan Zhang or Dengfeng Wang.

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Zhang, X., Wang, D., Ma, J. et al. Fluorinated Mg–Al Hydrotalcites Derived Basic Catalysts for Transesterification of Glycerol with Dimethyl Carbonate. Catal Lett 147, 1181–1196 (2017). https://doi.org/10.1007/s10562-017-2013-9

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  • DOI: https://doi.org/10.1007/s10562-017-2013-9

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