The emergence of porous liquids (PLs) opened opportunities to form unique antagonistic systems capable of fulfilling cascade reactions promoted by incompatible active sites in one pot, which is a long-term challenging subject in catalysis. Herein, unique bifunctional type III PL-based systems were facilely fabricated via assembly of zeolite nanosheets with ionic liquids. Rational structural design afforded PLs that feature high zeolite concentration, stable dispersion after 2 years, abundant cavity distribution, and involvement of antagonistic groups (acid and base sites) in separated and active form via steric hindrance control and electronic repulsion regulation. These unique properties worked cooperatively to fulfill the cascade deacetalization-Knoevenagel/Aldol condensation in one pot with superior catalytic efficiency outperforming the traditional systems. The key to success lies in the formation of bifunctional composites, transformation of zeolite from heterogeneous to homogeneous via surface modification, and rapid mass transfer ensured by the rigid porous architecture.

多孔液体（PLs）的出现为形成独特的拮抗系统提供了机会，该系统能够实现由不相容的活性位点在一锅中促进的级联反应，这是催化领域的一个长期具有挑战性的课题。在此，独特的基于双功能 III 型 PL 的系统通过沸石纳米片与离子液体的组装轻松制造。合理的结构设计使 PLs 具有沸石浓度高、2 年后分散稳定、空穴分布丰富、拮抗基团（酸和碱位点）通过空间位阻控制和电子排斥调节以分离和活性形式参与的特点。这些独特的特性协同作用，在一个锅中实现了级联脱缩醛-Knoevenagel/Aldol 缩合，具有优于传统系统的卓越催化效率。成功的关键在于双功能复合材料的形成、沸石通过表面改性从异质到均质的转变，以及由刚性多孔结构确保的快速传质。