Liqi Qiu, Tao Wang, Hongjun Liu, Arvind Ganesan, Errui Li, Kevin Michael Siniard, Jian Zhi Hu, Lilin He, Gergely Nagy, Alexander S Ivanov, Xin Wang, Leighanne C Gallington, Victoria Cooley, De-En Jiang, Shannon M Mahurin, Yong Wang, Zhenzhen Yang, Sheng Dai
Basic solutions are essential for gas-involved catalytic transformations, yet their ultralow free volume limits gas solubility and diffusivity. Engineering permanent porosity in such reactive liquids has remained a longstanding challenge. Here, we introduce a surface-sacrifice strategy that incorporates Brønsted-acidic zeolite nanocrystals into strong organic bases to create permanently porous reactive liquids. Stereochemically controlled acid-base neutralization at the external zeolite surface forms a thin ionic solvation shell that stabilizes the dispersion while fully preserving the internal microporosity and crystallinity of the zeolite framework. The resulting basic media exhibit persistent microporosity, confirmed by inert-gas sorption, 129Xe nuclear magnetic resonance, neutron scattering, and theoretical simulations. These porous liquids show significantly enhanced catalytic performance in CO2 conversion and hydrogenation reactions. The coexisting acidic and basic sites further enable antagonistic cascade catalysis within a single liquid phase. This surface-sacrifice approach provides a general route to introduce permanent porosity into reactive media, enabling boosted gas transformations.