摘要：In solid basic catalysis field,how to achieve optimized activity and desired stability through elaborate control over basic site properties remains a *** this work,taking advantage of the structure memory effect of layered double hydroxides(LDHs),rehydrated Ca4 Al1-x Gax-LDHs and Ca4 Al1-x Inx-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-Ca4 Al0.90Ga0.10-LDHs exhibits an extraordinarily-high catalytic activity(HPA yield:72%),which is to our best knowledge the highest level in this *** weak Br?nsted basic site,7-coordinated Ca-OH group,which serves as an active site,catalyzes the condensation process and promotes the product *** 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 *** 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.