Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites

Vera Bocharova; Nishani Jayakody; Jie Yang; Robert L. Sacci; Wei Yang; Shiwang Cheng; Benjamin Doughty; Steven Greenbaum; Seung Pyo Jeong; Ivan Popov; Sheng Zhao; Catalin Gainaru; Zaneta Wojnarowska

doi:10.1021/acsami.0c08323

Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites

Vera Bocharova, Nishani Jayakody, Jie Yang, Robert L. Sacci, Wei Yang, Shiwang Cheng, Benjamin Doughty, Steven Greenbaum, Seung Pyo Jeong, Ivan Popov, Sheng Zhao, Catalin Gainaru, Zaneta Wojnarowska

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

Ionic liquid (IL) properties, such as high ionic conductivity under ambient conditions combined with nontoxicity and nonflammability, make them important materials for future technologies. Despite high ion conductivity desired for battery applications, cation transport numbers in ILs are not sufficient enough to attain high power density batteries. Thus, developing novel approaches directed toward improvement of cation transport properties is required for the application of ILs in energy-storing devices. In this effort, we used various experimental techniques to demonstrate that the strategy of mixing ILs with ultrasmall (1.8 nm) nanoparticles (NPs) resulted in melt-processable composites with improved transport numbers for cations at room temperature. This significant enhancement in the transport number was attributed to the specific chemistry of NPs exhibiting a weaker cation and stronger anion coordination at ambient temperature. At high temperature, significantly weakened NP-anion associations promoted a liquid-like behavior of composites, highlighting the melt-processability of these composites. These results show that designing a reversible dynamic noncovalent NP-anion association controlled by the temperature may constitute an effective strategy to control ion diffusion. Our studies provide fundamental insights into mechanisms driving the charge transport and offer practical guidance for the design of melt-processable composites with an improved cation transport number under ambient conditions.

Original language	English
Pages (from-to)	31842-31851
Number of pages	10
Journal	ACS Applied Materials and Interfaces
Volume	12
Issue number	28
DOIs	https://doi.org/10.1021/acsami.0c08323
State	Published - Jul 15 2020

Funding

This work was supported by Laboratory Directed Research and Development program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. I.P. and R.L.C. acknowledge the partial financial support by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division for data analysis and FTIR measurements. B.D. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. N.J. and S.G. acknowledge support from the U.S. Office of Naval Research, grant # N00014-20-1-2186. C.G. acknowledges financial support from Deutsche Forschungsgemeinschaft under GA2680/1-1 project.

Funders	Funder number
Office of Naval Research	N00014-20-1-2186
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Laboratory Directed Research and Development
Chemical Sciences, Geosciences, and Biosciences Division
Deutsche Forschungsgemeinschaft	GA2680/1-1

Keywords

cation transport number
dynamic bonds
energy storage
ionic conductivity
nanocomposites

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10.1021/acsami.0c08323

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Bocharova, V., Jayakody, N., Yang, J., Sacci, R. L., Yang, W., Cheng, S., Doughty, B., Greenbaum, S., Jeong, S. P., Popov, I., Zhao, S., Gainaru, C., & Wojnarowska, Z. (2020). Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites. ACS Applied Materials and Interfaces, 12(28), 31842-31851. https://doi.org/10.1021/acsami.0c08323

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title = "Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites",

abstract = "Ionic liquid (IL) properties, such as high ionic conductivity under ambient conditions combined with nontoxicity and nonflammability, make them important materials for future technologies. Despite high ion conductivity desired for battery applications, cation transport numbers in ILs are not sufficient enough to attain high power density batteries. Thus, developing novel approaches directed toward improvement of cation transport properties is required for the application of ILs in energy-storing devices. In this effort, we used various experimental techniques to demonstrate that the strategy of mixing ILs with ultrasmall (1.8 nm) nanoparticles (NPs) resulted in melt-processable composites with improved transport numbers for cations at room temperature. This significant enhancement in the transport number was attributed to the specific chemistry of NPs exhibiting a weaker cation and stronger anion coordination at ambient temperature. At high temperature, significantly weakened NP-anion associations promoted a liquid-like behavior of composites, highlighting the melt-processability of these composites. These results show that designing a reversible dynamic noncovalent NP-anion association controlled by the temperature may constitute an effective strategy to control ion diffusion. Our studies provide fundamental insights into mechanisms driving the charge transport and offer practical guidance for the design of melt-processable composites with an improved cation transport number under ambient conditions.",

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author = "Vera Bocharova and Nishani Jayakody and Jie Yang and Sacci, {Robert L.} and Wei Yang and Shiwang Cheng and Benjamin Doughty and Steven Greenbaum and Jeong, {Seung Pyo} and Ivan Popov and Sheng Zhao and Catalin Gainaru and Zaneta Wojnarowska",

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Bocharova, V, Jayakody, N, Yang, J, Sacci, RL, Yang, W, Cheng, S, Doughty, B, Greenbaum, S, Jeong, SP, Popov, I, Zhao, S, Gainaru, C & Wojnarowska, Z 2020, 'Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites', ACS Applied Materials and Interfaces, vol. 12, no. 28, pp. 31842-31851. https://doi.org/10.1021/acsami.0c08323

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T1 - Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites

AU - Bocharova, Vera

AU - Jayakody, Nishani

AU - Yang, Jie

AU - Sacci, Robert L.

AU - Yang, Wei

AU - Cheng, Shiwang

AU - Doughty, Benjamin

AU - Greenbaum, Steven

AU - Jeong, Seung Pyo

AU - Popov, Ivan

AU - Zhao, Sheng

AU - Gainaru, Catalin

AU - Wojnarowska, Zaneta

PY - 2020/7/15

Y1 - 2020/7/15

N2 - Ionic liquid (IL) properties, such as high ionic conductivity under ambient conditions combined with nontoxicity and nonflammability, make them important materials for future technologies. Despite high ion conductivity desired for battery applications, cation transport numbers in ILs are not sufficient enough to attain high power density batteries. Thus, developing novel approaches directed toward improvement of cation transport properties is required for the application of ILs in energy-storing devices. In this effort, we used various experimental techniques to demonstrate that the strategy of mixing ILs with ultrasmall (1.8 nm) nanoparticles (NPs) resulted in melt-processable composites with improved transport numbers for cations at room temperature. This significant enhancement in the transport number was attributed to the specific chemistry of NPs exhibiting a weaker cation and stronger anion coordination at ambient temperature. At high temperature, significantly weakened NP-anion associations promoted a liquid-like behavior of composites, highlighting the melt-processability of these composites. These results show that designing a reversible dynamic noncovalent NP-anion association controlled by the temperature may constitute an effective strategy to control ion diffusion. Our studies provide fundamental insights into mechanisms driving the charge transport and offer practical guidance for the design of melt-processable composites with an improved cation transport number under ambient conditions.

AB - Ionic liquid (IL) properties, such as high ionic conductivity under ambient conditions combined with nontoxicity and nonflammability, make them important materials for future technologies. Despite high ion conductivity desired for battery applications, cation transport numbers in ILs are not sufficient enough to attain high power density batteries. Thus, developing novel approaches directed toward improvement of cation transport properties is required for the application of ILs in energy-storing devices. In this effort, we used various experimental techniques to demonstrate that the strategy of mixing ILs with ultrasmall (1.8 nm) nanoparticles (NPs) resulted in melt-processable composites with improved transport numbers for cations at room temperature. This significant enhancement in the transport number was attributed to the specific chemistry of NPs exhibiting a weaker cation and stronger anion coordination at ambient temperature. At high temperature, significantly weakened NP-anion associations promoted a liquid-like behavior of composites, highlighting the melt-processability of these composites. These results show that designing a reversible dynamic noncovalent NP-anion association controlled by the temperature may constitute an effective strategy to control ion diffusion. Our studies provide fundamental insights into mechanisms driving the charge transport and offer practical guidance for the design of melt-processable composites with an improved cation transport number under ambient conditions.

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KW - dynamic bonds

KW - energy storage

KW - ionic conductivity

KW - nanocomposites

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JF - ACS Applied Materials and Interfaces

IS - 28

ER -

Modulation of Cation Diffusion by Reversible Supramolecular Assemblies in Ionic Liquid-Based Nanocomposites

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