LAUSR

Bifunctional acid‐base catalysts have been developed by fabricating core‐shell faujasite@aqueous miscible organic‐layered double hydroxides (FAU@AMO‐LDHs) composites via the growth of AMO‐LDHs on zeolite surfaces. Interestingly, by adjusting the acid/base properties of the composites, the one‐pot synthesis of ethyl trans‐α‐cyanocinnamate via deacetalization‐Knoevenagel reaction can be achieved up to 90% yield. In contrast, almost no desired products can be observed in cases of isolated zeolites and AMO‐LDHs, demonstrating the synergistic effect of zeolites and AMO‐LDHs as acid‐base catalysts. These findings open up new perspectives of the development of tunable acid‐base zeolite@LDHs composites in an acid‐base tandem reaction, which can selectively produce ethyl trans‐α‐cyanocinnamate up to 90% yield.