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Herein, we propose a host\u2013guest complexation enhanced dissolution strategy for constructing Type II PLs from MOPs with record\u2010high concentration. Benefitting from host\u2013guest interactions between pillar[5]arene and\n                    <jats:italic>n<\/jats:italic>\n                    \u2010alkyl chains, a Type II PL (P5\u2010PL) is developed by dissolving apolar\n                    <jats:italic>n<\/jats:italic>\n                    \u2010dodecyl\u2010functionalized metal\u2013organic polyhedra (MOP\u201018) in polar liquid pillar[5]arene (P5\u2010L), exhibiting solubility much higher than all MOP\u2010based Type II PLs reported to date. MOP\u201018, being nonporous in the solid state because of molecular packing\u2010induced pore blockage, displays permanent molecular porosity when molecularly and randomly dispersed in P5\u2010L to form P5\u2010PL, as confirmed by experimental and simulation results. P5\u2010PL demonstrates excellent CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    separation capabilities, enabling the fabrication of mixed matrix membrane with superior CO\n                    <jats:sub>2<\/jats:sub>\n                    \/N\n                    <jats:sub>2<\/jats:sub>\n                    selectivity. This strategy can be extended to the fabrication of additional Type II PLs, showing its universality. This synergistic design concept integrating supramolecular chemistry with PLs not only overcomes traditional tedious covalent modification but also enables high compatibility between apolar cage solutes and polar solvents, affording PLs with high porosity, low volatility and viscosity, and programmable tunability.\n                  <\/jats:p>","DOI":"10.1002\/anie.202519288","type":"journal-article","created":{"date-parts":[[2025,10,17]],"date-time":"2025-10-17T12:56:58Z","timestamp":1760705818000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Synthesis of Type II Porous Liquids from Nonporous Metal\u2013Organic Polyhedra Enhanced by Host\u2013Guest Complexation"],"prefix":"10.1002","volume":"64","author":[{"given":"Zhaocong","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry MOE Laboratory of Mesoscopic Chemistry Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 P.R. 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