Citation: Huimin Wang, Weihan Bing, Chunyuan Chen, Yusen Yang, Ming Xu, Lifang Chen, Lei Zheng, Xiaolin Li, Xin Zhang, Jianjun Yin, Min Wei. Geometric effect promoted hydrotalcites catalysts towards aldol condensation reaction[J]. Chinese Journal of Catalysis, ;2020, 41(8): 1279-1287. doi: 10.1016/S1872-2067(20)63556-2 shu

Geometric effect promoted hydrotalcites catalysts towards aldol condensation reaction

Huimin Wang ^a, ,
Weihan Bing ^b ,
Chunyuan Chen ^a ,
Yusen Yang ^a ,
Ming Xu ^a ,
Lifang Chen ^a ,
Lei Zheng ^c ,
Xiaolin Li ^a ,
Xin Zhang ^a ,
Jianjun Yin ^d ,
Min Wei ^a

a State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
b China Tianchen Engineering Corporation Technology Research and Development Center, Tianjin 300400, China;
c Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China;
d SINOPEC Beijing Research Institute of Chemical Industry, Beijing 100013, China

Received Date: 12 November 2019
Revised Date: 27 December 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (21871021, 21521005 and 91741104), the National Key R&D Program of China (2017YFA0206804), and the Fundamental Research Funds for the Central Universities (buctylkxj01 and XK1802-6).

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 Ca₄Al_1-xGa_x-LDHs and Ca₄Al_1-xIn_x-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-Ca₄Al_0.90Ga_0.10-LDHs exhibits an extraordinarily-high catalytic activity (HPA yield:72%), which is to our best knowledge the highest level in this reaction. The weak Brönsted 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-Ca₄Al_0.90Ga_0.10-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.
- Solid basic catalyst,
- Geometric structure,
- Structural promoter,
- Aldol condensation,
- Reconstructed hydrotalcite material
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