Revolutionizing Porous Liquids: Stabilization and Structural Engineering Achieved by a Surface Deposition Strategy

Abstract Facile approaches capable of constructing stable and structurally diverse porous liquids (PLs) that can deliver high‐performance applications are a long‐standing, captivating, and challenging research area that requires significant attention. Herein, a facile surface deposition strategy is demonstrated to afford diverse type III‐PLs possessing ultra‐stable dispersion, external structure modification, and enhanced performance in gas storage and transformation by leveraging the expeditious and uniform precipitation of selected metal salts. The Ag(I) species‐modified zeolite nanosheets are deployed as the porous host to construct type III‐PLs with ionic liquids (ILs) containing bromide anion , leading to stable dispersion driven by the formation of AgBr nanoparticles. The as‐afforded type‐III PLs display promising performance in CO₂ capture/conversion and ethylene/ethane separation. Property and performance of the as‐produced PLs can be tuned by the cation structure of the ILs, which can be harnessed to achieve polarity reversal of the porous host via ionic exchange. The surface deposition procedure can be further extended to produce PLs from Ba(II)‐functionalized zeolite and ILs containing [SO₄]²⁻ anion driven by the formation of BaSO₄ salts. The as‐produced PLs are featured by well‐maintained crystallinity of the porous host, good fluidity and stability, enhanced gas uptake capacity, and attractive performance in small gas molecule utilization.