{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T19:25:41Z","timestamp":1788290741664,"version":"build-2803163510"},"reference-count":67,"publisher":"MDPI AG","issue":"1","license":[{"start":{"date-parts":[[2025,12,30]],"date-time":"2025-12-30T00:00:00Z","timestamp":1767052800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22271208"],"award-info":[{"award-number":["22271208"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Polymers"],"abstract":"<jats:p>Catalytic coacervates, or droplet reactors, represent a forefront research area in chemistry and materials science. Despite advancements in this field, challenges persist in achieving liquid\u2013liquid phase separation (LLPS) droplet compartmentalization and site-specific reactant recruitment\/localization for reaction catalysis, similar to those within biological systems. Herein, we describe the catalytic coacervates for aqueous photo-RAFT in dilution, focusing on the site-specific recruitment\/localization of ionized monomer with the aid of macromolecular crowding and confinement. Cooperative hydrogen-bonded interpolymer complexation (IPC) of imidazolium-copolymers initiates the ion-cluster formation. Further hierarchical inter-cluster complexation (ICC) leads to the LLPS droplet compartmentalization into charged dense-phase and neutral dilute-phase compartments. Site-specific recruitment and localization of the oppositely charged monomer into dense-phase compartments are achieved by salt-bridging molecular recognition. \u201cSubstantial DMA-dilution\u201d (that is, macromolecular crowding) results in sustainable dense-phase catalytic sites within dilute-phase crowding surroundings, enabling reaction catalysis in dilution (&lt;2% w\/w monomer) to 97% conversion in 12 min. These findings underscore the key roles of macromolecular crowding and confinement in the tailorable LLPS droplet compartmentalization and also the site-specific reactant recruitment\/localization essential for enzyme reaction catalysis, and provide practical guidelines for creating catalytic coacervates towards lifelike reaction functions.<\/jats:p>","DOI":"10.3390\/polym18010106","type":"journal-article","created":{"date-parts":[[2025,12,31]],"date-time":"2025-12-31T13:30:52Z","timestamp":1767187852000},"page":"106","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Site-Specific Recruitment, Localization of Ionized Monomer to Macromolecular Crowded Droplet Compartments Can Lead to Catalytic Coacervates for Photo-RAFT in Dilution"],"prefix":"10.3390","volume":"18","author":[{"given":"Wenjing","family":"Niu","sequence":"first","affiliation":[{"name":"State-Local Joint Engineering Laboratory for Novel Functional Polymer Materials, Jiangsu Key Laboratory of Advanced Functional Polymer Materials, Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiyu","family":"Wang","sequence":"additional","affiliation":[{"name":"State-Local Joint Engineering Laboratory for Novel Functional Polymer Materials, Jiangsu Key Laboratory of Advanced Functional Polymer Materials, Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ran","family":"Zhang","sequence":"additional","affiliation":[{"name":"State-Local Joint Engineering Laboratory for Novel Functional Polymer Materials, Jiangsu Key Laboratory of Advanced Functional Polymer Materials, Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuanli","family":"Cai","sequence":"additional","affiliation":[{"name":"State-Local Joint Engineering Laboratory for Novel Functional Polymer Materials, Jiangsu Key Laboratory of Advanced Functional Polymer Materials, Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2025,12,30]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"eaaf4382","DOI":"10.1126\/science.aaf4382","article-title":"Liquid phase condensation in cell physiology and disease","volume":"357","author":"Shin","year":"2017","journal-title":"Science"},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"53","DOI":"10.1146\/annurev-physchem-071819-113553","article-title":"Biomolecular phase separation: From molecular driving forces to macroscopic properties","volume":"71","author":"Dignon","year":"2020","journal-title":"Annu. 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