Adaptive ionic moieties for electrolyte structural design
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 66614 ] 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.
Authors
- Serena Cozzolino (ORCID: https://orcid.org/0000-0003-3528-5344)
- Liliana de Campo (ORCID: https://orcid.org/0000-0003-4799-2935)
- Daniel C. Morris (ORCID: https://orcid.org/0000-0002-8078-7848)
- Oliver S. Hammond (ORCID: https://orcid.org/0000-0002-5612-9343)
- Oleg N. Antzutkin (ORCID: https://orcid.org/0000-0003-1067-7990)
- Sergei B. Glavatskih (ORCID: https://orcid.org/0000-0002-8738-0047)
- Anja‐Verena Mudring (ORCID: https://orcid.org/0000-0002-2800-1684)
- Jason Brian Harper (ORCID: https://orcid.org/0000-0003-2722-8534)
- Guillaume Bousrez (ORCID: https://orcid.org/0000-0002-0265-7431)
- Sichao Li (ORCID: https://orcid.org/0000-0001-7195-1792)
- Mark William Rutland (ORCID: https://orcid.org/0000-0002-8935-8070)
- Andrew E. Whitten (ORCID: https://orcid.org/0000-0001-8856-3120)
- Andrew R. J. Nelson (ORCID: https://orcid.org/0000-0002-4548-3558)
- Stuart J. Brown (ORCID: https://orcid.org/0000-0002-3324-2829)
- Alexei Vorobiev (ORCID: https://orcid.org/0000-0003-3778-4948)
- Manishkumar Shimpi
Institutions
- École Centrale de Lyon (FR)
- Uppsala University (SE)
- HOGENT University of Applied Sciences and Arts (BE)
- Australian Nuclear Science and Technology Organisation (AU)
- Stockholm University (SE)
- Luleå University of Technology (SE)
- Aarhus University (DK)
- RISE Research Institutes of Sweden (SE)
- UNSW Sydney (AU)
- Ghent University (BE)
- University Hospital of Umeå (SE)
- Institut Laue-Langevin (FR)
- Wallenberg Wood Science Center (SE)
- Umkhuseli Innovation and Research Management (ZA)
- KTH Royal Institute of Technology (SE)
- Umeå University (SE)
- University of KwaZulu-Natal (ZA)
Publication Details
- Journal
- Science Advances
- Published
- 2026-09-25
- DOI
- https://doi.org/10.1126/sciadv.aeh0276
- Primary Topic
- Ionic liquids properties and applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00