A classical density functional theory for interfacial layering of ionic liquids

Wu, Jianzhong; Jiang, Tao; Jiang, Deen; Jin, Zhehui; Henderson, Douglous

doi:10.1039/c1sm06089a

Title: A classical density functional theory for interfacial layering of ionic liquids

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Abstract

Ionic liquids have attracted much recent theoretical interest for broad applications as environmentally-friendly solvents in separation and electrochemical processes. Because of the intrinsic complexity of organic ions and strong electrostatic correlations, the electrochemical properties of ionic liquids often defy the descriptions of conventional mean-field methods including the venerable, and over-used, Gouy-Chapman-Stern (GCS) theory. Classical density functional theory (DFT) has proven to be useful in previous studies of the electrostatic properties of aqueous electrolytes but until recently it has not been applied to ionic liquids. Here we report predictions from the DFT on the interfacial properties of ionic liquids near neutral or charged surfaces. By considering the molecular size, topology, and electrostatic correlations, we have examined major factors responsible for the unique features of electric-double layers of ionic-liquid including formation of long-range and alternating structures of cations and anions at charged surfaces.

Authors:

Wu, Jianzhong ^[1]; Jiang, Tao ^[2]; Jiang, Deen ^[3]; Jin, Zhehui ^[1]; Henderson, Douglous ^[4]

University of California, Riverside
California Energy Commission
ORNL
Brigham Young University

Publication Date:: Sat Jan 01 00:00:00 EST 2011

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

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1033536

DOE Contract Number:: DE-AC05-00OR22725

Resource Type:: Journal Article

Journal Name:: Soft Matter

Additional Journal Information:: Journal Volume: 7; Journal Issue: 23; Journal ID: ISSN 1744-683X

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ANIONS; CATIONS; ELECTROSTATICS; DENSITY FUNCTIONAL METHOD; MOLECULAR STRUCTURE; MOLTEN SALTS; SOLVENTS; TOPOLOGY

Citation Formats


                    Wu, Jianzhong, Jiang, Tao, Jiang, Deen, Jin, Zhehui, and Henderson, Douglous. A classical density functional theory for interfacial layering of ionic liquids.  United States: N. p., 2011. 
        Web.  doi:10.1039/c1sm06089a.

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                    Wu, Jianzhong, Jiang, Tao, Jiang, Deen, Jin, Zhehui, & Henderson, Douglous. A classical density functional theory for interfacial layering of ionic liquids.  United States.  https://doi.org/10.1039/c1sm06089a

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                    Wu, Jianzhong, Jiang, Tao, Jiang, Deen, Jin, Zhehui, and Henderson, Douglous. 2011.  
        "A classical density functional theory for interfacial layering of ionic liquids".  United States.  https://doi.org/10.1039/c1sm06089a.

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@article{osti_1033536,

  title        = {A classical density functional theory for interfacial layering of ionic liquids},

  author       = {Wu, Jianzhong and Jiang, Tao and Jiang, Deen and Jin, Zhehui and Henderson, Douglous},

  abstractNote = {Ionic liquids have attracted much recent theoretical interest for broad applications as environmentally-friendly solvents in separation and electrochemical processes. Because of the intrinsic complexity of organic ions and strong electrostatic correlations, the electrochemical properties of ionic liquids often defy the descriptions of conventional mean-field methods including the venerable, and over-used, Gouy-Chapman-Stern (GCS) theory. Classical density functional theory (DFT) has proven to be useful in previous studies of the electrostatic properties of aqueous electrolytes but until recently it has not been applied to ionic liquids. Here we report predictions from the DFT on the interfacial properties of ionic liquids near neutral or charged surfaces. By considering the molecular size, topology, and electrostatic correlations, we have examined major factors responsible for the unique features of electric-double layers of ionic-liquid including formation of long-range and alternating structures of cations and anions at charged surfaces.},

  doi          = {10.1039/c1sm06089a},

  url          = {https://www.osti.gov/biblio/1033536},
  journal      = {Soft Matter},

  issn         = {1744-683X},

  number       = 23,

  volume       = 7,

  place        = {United States},

  year         = {Sat Jan 01 00:00:00 EST 2011},

  month        = {Sat Jan 01 00:00:00 EST 2011}

}

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