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The variety of layered uranyl hydroxides (LUHs) remains limited; only four neutral LUH phases have been structurally confirmed. Herein, we report the synthesis and characterization of the first charged LUH, [BMIM]2[(UO2)5(OH)12(H2O)2] (BMIM-UOH), which represents the fifth confirmed LUH phase. In BMIM-UOH, pentagonal-bipyramidal uranyl units are interconnected to vertex-sharing [(UO2)5(\u03bc2-OH)12] ({U5}) clusters, which further link to form extended two-dimensional anionic sheets, with ionic liquid cations serving as interlayer counterions. The resulting uranyl hydroxide layer exhibits a new anion topology that has not been observed in other uranyl compounds. Notably, the ionic liquid cations occupy the interlayer galleries, where they stabilize the layered structures through electrostatic interactions and hydrogen bonding. This structure represents a rare example of LUHs, highlighting the role of ionic liquids in modulating actinyl hydrolysis and assembling layered materials.<\/jats:p>","DOI":"10.1021\/acs.inorgchem.6c02887","type":"journal-article","created":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T14:01:53Z","timestamp":1789394513000},"page":"22214-22219","source":"Crossref","is-referenced-by-count":0,"title":["Layered Uranyl\nHydroxide Assembled from Negatively\nCharged Host Layers and Interlayer Cations through Noncovalent Interactions"],"prefix":"10.1021","volume":"65","author":[{"given":"Lei","family":"Chen","sequence":"first","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7099-2103","authenticated-orcid":true,"given":"Junyi","family":"Li","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Penglin","family":"Dou","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunzhe","family":"Ma","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lechen","family":"Ma","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Boyang","family":"Song","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-1489-7708","authenticated-orcid":true,"given":"Hailong","family":"Zhang","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1842-339X","authenticated-orcid":true,"given":"Yaxing","family":"Wang","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1526-1102","authenticated-orcid":true,"given":"Shuao","family":"Wang","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, China, 215123"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,14]]},"reference":[{"key":"2026092809215797500_cit1","doi-asserted-by":"publisher","first-page":"14503","DOI":"10.1021\/ja104964x","article-title":"Understanding the Structure and Formation\nof Uranyl Peroxide Nanoclusters by Quantum Chemical Calculations","volume":"132","author":"Vlaisavljevich","year":"2010","journal-title":"J. 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Alloys Compd."},{"key":"2026092809215797500_cit28","doi-asserted-by":"publisher","first-page":"15854","DOI":"10.1039\/D0DT02944K","article-title":"Uranyl Oxide Hydrate\nFrameworks with Lanthanide Ions","volume":"49","author":"Lu","year":"2020","journal-title":"Dalt. Trans."},{"key":"2026092809215797500_cit29","doi-asserted-by":"publisher","first-page":"425","DOI":"10.31635\/ccschem.020.202000152","article-title":"Stabilization\nof Plutonium(V) within a Crown Ether Inclusion Complex","volume":"2","author":"Wang","year":"2020","journal-title":"CCS Chem."},{"key":"2026092809215797500_cit30","doi-asserted-by":"publisher","first-page":"5330","DOI":"10.1021\/acs.cgd.7b00838","article-title":"Spectral Analysis\nof the Uranyl Squarate and Croconate System: Evaluating Differences\nbetween the Solution and Solid-State Phases","volume":"17","author":"Basile","year":"2017","journal-title":"Cryst. Growth Des."},{"key":"2026092809215797500_cit31","doi-asserted-by":"publisher","first-page":"608","DOI":"10.1039\/C9DT04000E","article-title":"Solid State Characterization of Oxidized Actinides\nCo-Crystallized with Uranyl Nitrate Hexahydrate","volume":"49","author":"Einkauf","year":"2020","journal-title":"Dalt. Trans."},{"key":"2026092809215797500_cit32","doi-asserted-by":"publisher","first-page":"9706","DOI":"10.1021\/acs.inorgchem.4c00801","article-title":"Semiconductive\nBehavior and Photoconductivity\nof Uranyl Dithiophosphinate Single Crystal","volume":"63","author":"Wang","year":"2024","journal-title":"Inorg. Chem."},{"key":"2026092809215797500_cit33","doi-asserted-by":"publisher","first-page":"13161","DOI":"10.1021\/jacs.3c01968","article-title":"Near-Unity Energy Transfer\nfrom Uranyl to Europium in a Heterobimetallic Organic Framework with\nRecord-Breaking Quantum Yield","volume":"145","author":"Zhang","year":"2023","journal-title":"J. Am. Chem.\nSoc."},{"key":"2026092809215797500_cit34","doi-asserted-by":"publisher","first-page":"8455","DOI":"10.1021\/acs.inorgchem.2c00233","article-title":"Stability of Studtite in Saline Solution:\nIdentification of Uranyl\u2013Peroxo\u2013Halo Complex","volume":"61","author":"Li","year":"2022","journal-title":"Inorg. Chem."},{"key":"2026092809215797500_cit35","doi-asserted-by":"publisher","first-page":"5280","DOI":"10.1021\/ic00051a021","article-title":"Aqueous Uranium\nComplexes. 2. Raman\nSpectroscopic Study of the Complex Formation of the Dioxouranium(VI)\nIon with a Variety of Inorganic and Organic Ligands","volume":"31","author":"Nguyen-Trung","year":"1992","journal-title":"Inorg. Chem."},{"key":"2026092809215797500_cit36","doi-asserted-by":"publisher","first-page":"15041","DOI":"10.1002\/anie.202103039","article-title":"Isolation and Reactivity of Uranyl\nSuperoxide","volume":"60","author":"Kravchuk","year":"2021","journal-title":"Angew. Chem., Int. 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