4.7 Article

Geometric effect promoted hydrotalcites catalysts towards aldol condensation reaction

期刊

CHINESE JOURNAL OF CATALYSIS
卷 41, 期 8, 页码 1279-1287

出版社

SCIENCE PRESS
DOI: 10.1016/S1872-2067(20)63556-2

关键词

Solid basic catalyst; Geometric structure; Structural promoter; Aldol condensation; Reconstructed hydrotalcite material

资金

  1. National Natural Science Foundation of China [21871021, 21521005, 91741104]
  2. National Key R&D Program of China [2017YFA0206804]
  3. Fundamental Research Funds for the Central Universities [buctylkxj01, XK1802-6]

向作者/读者索取更多资源

In solid basic catalysis field, how to achieve optimized activity and desired stability through elaborate control over basic site properties remains a challenge. In this work, taking advantage of the structure memory effect of layered double hydroxides (LDHs), rehydrated Ca4Al1-xGax-LDHs and Ca4Al1-xInx-LDHs catalysts were prepared and applied in aldol condensation reaction that isobutyraldehyde (IBD) reacts with formaldehyde (FA) to obtain hydroxypivalaldehyde (HPA). Notably, the resulting re-Ca4Al0.90Ga0.10-LDHs exhibits an extraordinarily-high catalytic activity (HPA yield: 72%), which is to our best knowledge the highest level in this reaction. The weak Bronsted basic site, 7-coordinated Ca-OH group, which serves as an active site, catalyzes the condensation process and promotes the product desorption. Studies on structure-property correlations demonstrate that Ga as a structural promoter induces a moderate expansion of the laminate lattice, which results in a significant increase in the concentration of weak basic sites in re-Ca4Al0.90Ga0.10-LDHs, accounting for its high catalytic activity. This work illuminates that geometric structure of basic active sites can be tuned via introducing catalyst additive, which leads to a largely improved performance of hydrotalcite solid basic catalysts towards aldol condensation reaction. (C) 2020, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

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