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Here, we report a solvation\u2010gradient membrane prepared via reaction\u2010diffusion\u2010coupled interfacial polymerization between piperazine and 1,3,5\u2010tris(bromomethyl)benzene. The resulting membrane comprised a dense outer selective layer approximately 35\u00a0nm thick (with a transport pore size of approximately 6 \u00c5) and an NH\u2010rich inner layer approximately 400\u00a0nm thick. The outer layer imposes a high entry\/desolvation barrier on large ions, thereby inhibiting their transport, whereas the NH\u2010rich region supports rapid OH\n                    <jats:sup>\u2212<\/jats:sup>\n                    transport through re\u2010solvation and hydrogen\u2010bond reorganization. This depth\u2010dependent architecture spatially separates ferricyanide rejection from hydroxide conduction. Depth\u2010resolved spectroscopy and molecular dynamics simulations supported a depth\u2010dependent solvation environment and revealed stronger water\/OH\n                    <jats:sup>\u2212<\/jats:sup>\n                    interactions in the NH\u2010rich region. Optimization of poly(tertiary amine) (PTA) membranes achieved low Fe(CN)\n                    <jats:sub>6<\/jats:sub>\n                    <jats:sup>3\u2212<\/jats:sup>\n                    permeability (8.07 \u00d7 10\n                    <jats:sup>\u22127<\/jats:sup>\n                    cm\n                    <jats:sup>2<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and OH\n                    <jats:sup>\u2212<\/jats:sup>\n                    conductivity (41.08 mS cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), enabling an alkaline zinc\u2010iron flow battery to achieve an energy efficiency of 89.94% at 80\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and stable cycling for over 800\u00a0h. This study suggests depth\u2010dependent solvation regulation as a useful design principle for alleviating the selectivity\u2010conductivity trade\u2010off in electrochemical membranes.\n                  <\/jats:p>","DOI":"10.1002\/anie.9300778","type":"journal-article","created":{"date-parts":[[2026,8,23]],"date-time":"2026-08-23T17:45:12Z","timestamp":1787507112000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Solvation\u2010Gradient Thin\u2010Film Composite Membranes Decouple Ferricyanide Rejection From Hydroxide Conduction in Alkaline Zinc\u2013Iron Flow Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Junhua","family":"Li","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3097-9363","authenticated-orcid":false,"given":"Dan","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yijing","family":"Dai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zilin","family":"Zhao","sequence":"additional","affiliation":[{"name":"Suzhou Institute for Advanced Research University of Science and Technology of China  Suzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuzhang","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0429-300X","authenticated-orcid":false,"given":"Jian","family":"Jin","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,23]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ensm.2024.103226"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2025.101976"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202300779"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202405436"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010024\u201008140\u20102"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201506199"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202503110"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010019\u201013704\u20102"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.4c00301"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/app.35524"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202417994"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2022.08.043"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202500931"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c06641"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.166471"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6SC02865A"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.5c04520"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/aic.18038"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.3c02666"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.progpolymsci.2021.101451"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.memsci.2020.118507"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3TA05159E"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202001382"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.watres.2025.123337"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202504515"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.166111"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature00797"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcb.5c03199"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010022\u201033868\u20108"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.adr5374"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8TA10651G"}],"container-title":["Angewandte Chemie International Edition"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.9300778","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/anie.9300778","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/anie.9300778","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T15:50:12Z","timestamp":1791647412000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/anie.9300778"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,23]]},"references-count":31,"journal-issue":{"issue":"42","published-print":{"date-parts":[[2026,10,12]]}},"alternative-id":["10.1002\/anie.9300778"],"URL":"https:\/\/doi.org\/10.1002\/anie.9300778","archive":["Portico"],"relation":{},"ISSN":["1433-7851","1521-3773"],"issn-type":[{"value":"1433-7851","type":"print"},{"value":"1521-3773","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,23]]},"assertion":[{"value":"2026-06-02","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-08-13","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-08-23","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e9300778"}}