Self-Assembly Versus Surface Charge: Interfacial Response of Ionic Liquids
Abstract The bulk and surface charge-driven interfacial structuring of two 1-decyl-3-methylimidazolium (C10C1Im) orthoborate ionic liquids (ILs), dispersed at various concentrations in the polar aprotic solvent propylene carbonate (PC), were studied using small angle neutron scattering (SANS) and neutron reflectivity (NR). In the bulk, the larger bis(mandelato)borate anion reduced the self-assembly capabilities of the blend relative to bis(oxalate)borate. At a charged Au electrode interface, a distinct interfacial region was detected in all the IL mixtures studied, which was attributed to two interdigitated bilayers of the cation, containing intercalated anions and solvent, and with bulk IL concentration dependence. Under applied potential, higher concentrations showed clear anion effects on the electro-structuring, whereas dilute solutions were anion independent. The complex bulk and electro-responsive interfacial structuring of such self-assembling IL systems in polar media are pertinent to the application of ILs as designer electrolytes for advanced electrochemical technologies, including next-generation batteries and control over the electrical double layer in capacitors.
Authors
- Liliana de Campo (ORCID: https://orcid.org/0000-0003-4799-2935)
- Oliver S. Hammond (ORCID: https://orcid.org/0000-0002-5612-9343)
- Sergei Glavatskih (ORCID: https://orcid.org/0000-0002-8738-0047)
- Anja‐Verena Mudring (ORCID: https://orcid.org/0000-0002-2800-1684)
- Erik Bergendal (ORCID: https://orcid.org/0000-0001-9197-4676)
- Georgia A. Pilkington (ORCID: https://orcid.org/0000-0002-9815-8329)
- Akepati Bhaskar Reddy (ORCID: https://orcid.org/0000-0002-2716-8810)
- Mark W. Rutland (ORCID: https://orcid.org/0000-0002-8935-8070)
- Rebecca J. L. Welbourn (ORCID: https://orcid.org/0000-0002-4254-5354)
- Andrew Nelson (ORCID: https://orcid.org/0000-0002-4548-3558)
- Stuart J. Brown
- Sichao Li (ORCID: https://orcid.org/0000-0002-0097-6754)
- Anna Oleshkevych
- Manishkumar R. Shimpi
Institutions
- École Centrale de Lyon (FR)
- HOGENT University of Applied Sciences and Arts (BE)
- Rutherford Appleton Laboratory (GB)
- Australian Nuclear Science and Technology Organisation (AU)
- Stockholm University (SE)
- Luleå University of Technology (SE)
- Aarhus University (DK)
- European Spallation Source (SE)
- RISE Research Institutes of Sweden (SE)
- Ghent University Hospital (BE)
- UNSW Sydney (AU)
- Ghent University (BE)
- KTH Royal Institute of Technology (SE)
- Umeå University (SE)
Publication Details
- Journal
- Langmuir
- Published
- 2026-09-16
- DOI
- https://doi.org/10.1021/acs.langmuir.6c03265
- Primary Topic
- Ionic liquids properties and applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00