Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces

Mao, Xianwen; Brown, Paul; Červinka, Ctirad; Hazell, Gavin; Li, Hua; Ren, Yinying; Chen, Di; Atkin, Rob; Eastoe, Julian; Grillo, Isabelle; Padua, Agilio. A.  H.; Costa Gomes, Margarida. F.; Hatton, T. Alan

doi:10.1038/s41563-019-0449-6

Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces

Journal Article · Mon Aug 12 00:00:00 EDT 2019 · Nature Materials

DOI:https://doi.org/10.1038/s41563-019-0449-6· OSTI ID:1594997

^[1]; Brown, Paul ^[2]; Červinka, Ctirad ^[3]; Hazell, Gavin ^[4]; Li, Hua ^[5]; Ren, Yinying ^[2]; Chen, Di ^[6]; Atkin, Rob ^[5]; Eastoe, Julian ^[7]; Grillo, Isabelle ^[8]; Padua, Agilio. A. H. ^[9]; ^[9]; ^[2]

Cornell Univ., Ithaca, NY (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Ecole Normale Supérieure de Lyon (France); Centre National de la Recherche Scientifique (CNRS), Lyon (France); Univ. of Chemistry and Technology, Prague (Czech Republic)
Univ. of Chester (United Kingdom)
Univ. of Western Australia, Perth, WA (Australia)
Stanford Univ., CA (United States)
Univ. of Bristol (United Kingdom)
Inst. Laue–Langevin, Grenoble (France)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Ecole Normale Supérieure de Lyon (France); Centre National de la Recherche Scientifique (CNRS), Lyon (France)

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. We report that 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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Czech Science Foundation; Science and Technology Facilities Council (STFC) (United Kingdom); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1594997

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 12 Vol. 18; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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