Effect of SiO 2 amount on heterogeneous base catalysis of SiO 2 @Mg-Al layered double hydroxide

The effects of SiO amount on the base catalysis of highly active finely crystallized Mg-Al type layered double hydroxides prepared by the co-precipitation method with coexistence of SiO spheres, denoted as SiO @LDHs, were investigated. With the Si/(Mg + Al) atomic ratios of 0-0.50, the highest activ...

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Veröffentlicht in:RSC advances 2018-08, Vol.8 (49), p.28024-28031
Hauptverfasser: Shirotori, Mahiro, Nishimura, Shun, Ebitani, Kohki
Format: Artikel
Sprache:eng
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Zusammenfassung:The effects of SiO amount on the base catalysis of highly active finely crystallized Mg-Al type layered double hydroxides prepared by the co-precipitation method with coexistence of SiO spheres, denoted as SiO @LDHs, were investigated. With the Si/(Mg + Al) atomic ratios of 0-0.50, the highest activity for the Knoevenagel condensation was observed in the case of Si/(Mg + Al) = 0.17, as the reaction rate of 171.1 mmol g(cat) h . The base activity increased concomitantly with decreasing LDH crystallite size up to Si/(Mg + Al) atomic ratio of 0.17. However, above the Si/(Mg + Al) atomic ratio of 0.17, the reaction rate and TOF were decreased although the total base amount was increased. Results of TEM-EDS and Si CP-MAS NMR suggest that the co-existing SiO causes advantages for dispersion and reduction of the LDH crystallite to improve the base catalysis of SiO @Mg-Al LDH, whereas the excess SiO species unfortunately poisons the highly active sites on the finely crystallized LDH crystals above a Si/(Mg + Al) atomic ratio of 0.17. According to these results, we inferred that the amount of spherical SiO seeds in the co-precipitation method is an important factor to increase the base catalysis of SiO @LDHs; the control of Si/(Mg + Al) atomic ratio is necessary to avoid the poisoning of highly active base sites on the LDH crystal.
ISSN:2046-2069
2046-2069
DOI:10.1039/c8ra04925d