Interfacial ionic 'liquids': connecting static and dynamic structures

Uysal, Ahmet; Zhou, Hua; Feng, Guang; Lee, Sang Soo; Li, Song; Cummings, Peter T.; Fulvio, Pasquale F.; Dai, Sheng; McDonough, John K.; Gogotsi, Yury G.; Fenter, Paul

doi:10.1088/0953-8984/27/3/032101

Title: Interfacial ionic 'liquids': connecting static and dynamic structures

Journal Article · Fri Dec 05 00:00:00 EST 2014 · Journal of Physics. Condensed Matter

DOI:https://doi.org/10.1088/0953-8984/27/3/032101· OSTI ID:1286835

Uysal, Ahmet ^[1]; Zhou, Hua ^[1]; Feng, Guang ^[2]; Lee, Sang Soo ^[1]; Li, Song ^[2]; Cummings, Peter T. ^[2]; Fulvio, Pasquale F. ^[3]; Dai, Sheng ^[3]; McDonough, John K. ^[4]; Gogotsi, Yury G. ^[4]; Fenter, Paul ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)
Vanderbilt Univ., Nashville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Drexel Univ., Philadelphia, PA (United States)

It is well known that room temperature ionic liquids (RTILs) often adopt a charge-separated layered structure, i.e. with alternating cation- and anion-rich layers, at electrified interfaces. However, the dynamic response of the layered structure to temporal variations in applied potential is not well understood. For this research, we used in situ, real-time x-ray reflectivity to study the potential-dependent electric double layer (EDL) structure of an imidazolium-based RTIL on charged epitaxial graphene during potential cycling as a function of temperature. The results suggest that the graphene–RTIL interfacial structure is bistable in which the EDL structure at any intermediate potential can be described by the combination of two extreme-potential structures whose proportions vary depending on the polarity and magnitude of the applied potential. This picture is supported by the EDL structures obtained by fully atomistic molecular dynamics simulations at various static potentials. Lastly, the potential-driven transition between the two structures is characterized by an increasing width but with an approximately fixed hysteresis magnitude as a function of temperature. The results are consistent with the coexistence of distinct anion- and cation-adsorbed structures separated by an energy barrier (~0.15 eV).

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1286835

Journal Information:: Journal of Physics. Condensed Matter, Vol. 27, Issue 3; ISSN 0953-8984

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 71 works

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