Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces
Authors
Mao, XianwenBrown, Paul
Cervinka, Citrad
Hazell, Gavin
Li, Hua
Ren, Yinying
Chen, Di
Atkin, Rob
Eastoe, Julian
Grillo, Isabelle
Agilio, Padua
Costa-Gomes, Mragarida
Hatton, Alan
Affiliation
Cornell University; Massachusetts Institute of Technology; Laboratoire de Chimie, Ecole Normale Supérieure de Lyon; University of Chemistry and Technology; University of Chester; University of Western Australia; Stanford University; University of Bristol; Institut Laue–LangevinPublication Date
2019-08-12
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Driven by the potential applications of ionic liquids (ILs) in many emerging electrochemical technologies, recent research efforts have been directed at understanding the complex ion ordering in these systems, to uncover novel energy storage mechanisms at IL–electrode interfaces. Here, we discover that surface-active ILs (SAILs), which contain amphiphilic structures inducing self-assembly, exhibit enhanced charge storage performance at electrified surfaces. Unlike conventional non amphiphilic ILs, for which ion distribution is dominated by Coulombic interactions, SAILs exhibit significant and competing van der Waals interactions owing to the non-polar surfactant tails, leading to unusual interfacial ion distributions. We reveal that, at an intermediate degree of electrode polarization, SAILs display optimum performance, because the low-charge-density alkyl tails are effectively excluded from the electrode surfaces, whereas the formation of non-polar domains along the surface suppresses undesired overscreening effects. This work represents a crucial step towards understanding the unique interfacial behaviour and electrochemical properties of amphiphilic liquid systems showing long-range ordering, and offers insights into the design principles for high-energy-density electrolytes based on spontaneous self-assembly behaviour.Citation
Mao, X., Brown, P., Cervinka, C., Hazell, G., Li, H., Ren, Y., Chen, D., Atkin, R., Eastoe, J., Grillo, I., Padua, A. A. H., Gomes, M. F. C. & Hatton, T. A. (2019). Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces. Nature Materials, 18, 1350–1357. https://doi.org/10.1038/s41563-019-0449-6Publisher
Nature ResearchJournal
Nature MaterialsAdditional Links
https://www.nature.com/articles/s41563-019-0449-6Type
ArticleLanguage
enISSN
1476-1122EISSN
1476-4660ae974a485f413a2113503eed53cd6c53
10.1038/s41563-019-0449-6
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Except where otherwise noted, this item's license is described as http://creativecommons.org/licenses/by-nc-nd/4.0/