Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition

doi:10.1016/j.molliq.2017.10.128

Title: Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition

Abstract

The energy density of an electric double layer (EDL) capacitor, a type of supercapacitor, depends on the ion distribution within the micropores of electrodes that are typically made of amorphous carbon. By using coarse-grained models and the classical density functional theory, we investigate the distributions of ionic species among different idealized nanopores in contact with an asymmetric ionic liquid mixture and the effects of the bulk electrolyte composition on capacitive energy storage. We find that a charged pore is always small-ion selective, provided all ions have the same valence and similar non-electrostatic interactions. While small ions enhance both the EDL capacitance and the accessibility of micropores, an ionic mixture containing ions of different sizes may yield a capacitance higher than those corresponding to pure ionic liquids. Furthermore, the increased capacitance may be attributed to more efficient ion packing near the charged surface. At certain conditions, the improvement is on a par with the anomalous capacitance rise for pure ionic liquids in electrodes with ultranarrow pores.

Authors:

^[1];

^[2]; Henderson, Douglas ^[3]; Wu, Jianzhong ^[1]

Univ. of California, Riverside, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Brigham Young Univ., Provo, UT (United States)

Publication Date:: 2017-11-03

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1557520

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Molecular Liquids

Additional Journal Information:: Journal Volume: 270; Journal Issue: C; Journal ID: ISSN 0167-7322

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Porous electrodes; Capacitance; Ionic-liquid mixtures; EDL structure; Ion selectivity; Classical density functional theory

Citation Formats


                    Neal, Justin N., Wesolowski, David J., Henderson, Douglas, and Wu, Jianzhong. Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition.  United States: N. p., 2017. 
        Web.  doi:10.1016/j.molliq.2017.10.128.

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                    Neal, Justin N., Wesolowski, David J., Henderson, Douglas, & Wu, Jianzhong. Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition.  United States.  doi:10.1016/j.molliq.2017.10.128.

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                    Neal, Justin N., Wesolowski, David J., Henderson, Douglas, and Wu, Jianzhong. Fri .  
        "Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition".  United States.  doi:10.1016/j.molliq.2017.10.128.  https://www.osti.gov/servlets/purl/1557520.

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@article{osti_1557520,

  title        = {Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition},

  author       = {Neal, Justin N. and Wesolowski, David J. and Henderson, Douglas and Wu, Jianzhong},

  abstractNote = {The energy density of an electric double layer (EDL) capacitor, a type of supercapacitor, depends on the ion distribution within the micropores of electrodes that are typically made of amorphous carbon. By using coarse-grained models and the classical density functional theory, we investigate the distributions of ionic species among different idealized nanopores in contact with an asymmetric ionic liquid mixture and the effects of the bulk electrolyte composition on capacitive energy storage. We find that a charged pore is always small-ion selective, provided all ions have the same valence and similar non-electrostatic interactions. While small ions enhance both the EDL capacitance and the accessibility of micropores, an ionic mixture containing ions of different sizes may yield a capacitance higher than those corresponding to pure ionic liquids. Furthermore, the increased capacitance may be attributed to more efficient ion packing near the charged surface. At certain conditions, the improvement is on a par with the anomalous capacitance rise for pure ionic liquids in electrodes with ultranarrow pores.},

  doi          = {10.1016/j.molliq.2017.10.128},

  journal      = {Journal of Molecular Liquids},

  number       = C,

  volume       = 270,

  place        = {United States},

  year         = {2017},

  month        = {11}

}

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DOI: 10.1016/j.molliq.2017.10.128

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Works referencing / citing this record:

Reduced Faradaic Contributions and Fast Charging of Nanoporous Carbon Electrodes in a Concentrated Sodium Nitrate Aqueous Electrolyte for Supercapacitors
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Abbas, Qamar; Gollas, Bernhard; Presser, Volker
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Abbas, Qamar; Gollas, Bernhard; Presser, Volker
Energy Technology, Vol. 7, Issue 9
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A first-principles roadmap and limits to design efficient supercapacitor electrode materials
journal, January 2019

Ali, Basant A.; Allam, Nageh K.
Physical Chemistry Chemical Physics, Vol. 21, Issue 32
DOI: 10.1039/c9cp02614b

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Title: Electric double layer capacitance for ionic liquids in nanoporous electrodes: Effects of pore size and ion composition

Abstract

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