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Adv."],"published-print":{"date-parts":[[2026,9,25]]},"abstract":"<jats:p>\n                    Ionic liquids (ILs) are now an established and ubiquitous material class. In energy applications and electroresponsive lubrication, their interfacial self-assembly is crucial for their properties. This in turn is determined by chemical structure and a local hierarchy of Coulombic, van der Waals, and solvophobic interactions. We hypothesize that delocalization of the ionic charge permits the Coulombic interactions to adapt to other self-assembly imperatives, promoting both bulk and interfacial self-assembly structures and enhancing double layer responses. Novel chelated bis(catecholato)borate anion architectures are introduced, with [P\n                    <jats:sub>66614<\/jats:sub>\n                    ] cations. Small\/wide-angle x-ray scattering of the ILs indicates pronounced cation assemblies. In the electrolyte solvent propylene carbonate, small-angle neutron scattering shows marked anion-dependent self-assembly modulation. Neutron reflectivity reveals analogous response in the electrochemical double layer; the catechols form thicker and more electroresponsive interfacial layers. Density functional theory calculations demonstrate electronic resonance, modulating the anion polarizability. This direct self-assembly control broadly affects electrochemistry, lubrication, and formulation design.\n                  <\/jats:p>","DOI":"10.1126\/sciadv.aeh0276","type":"journal-article","created":{"date-parts":[[2026,9,25]],"date-time":"2026-09-25T17:58:53Z","timestamp":1790359133000},"update-policy":"https:\/\/doi.org\/10.34133\/aaas_crossmark","source":"Crossref","is-referenced-by-count":0,"title":["Adaptive ionic moieties for electrolyte structural design"],"prefix":"10.1126","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5612-9343","authenticated-orcid":true,"given":"Oliver S.","family":"Hammond","sequence":"first","affiliation":[{"name":"European Spallation Source, Data Management &amp; Scientific Computing, Asmussens All\u00e9 305, Kongens Lyngby 2800, Hovedstaden, Denmark."},{"name":"Division of Surface and Corrosion Science, KTH Royal Institute of Technology, Brinellv\u00e4gen 8, Stockholm 10044, Stockholms l\u00e4n, Sweden."},{"name":"Department of 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