Single Ion Conducting Hairy Nanoparticle Additive to Improve Cycling Stability of Solid Polymer Electrolytes

Vera Bocharova; Xi Chelsea Chen; Seung Pyo Jeong; Zhengping Zhou; Robert L. Sacci; Jong K. Keum; Catalin Gainaru; Md Anisur Rahman; Ritu Sahori; Xiao Guang Sun; Pengfei Cao; Andrew Westover

doi:10.1021/acsaem.3c01106

Single Ion Conducting Hairy Nanoparticle Additive to Improve Cycling Stability of Solid Polymer Electrolytes

Vera Bocharova, Xi Chelsea Chen, Seung Pyo Jeong, Zhengping Zhou, Robert L. Sacci, Jong K. Keum, Catalin Gainaru, Md Anisur Rahman, Ritu Sahori, Xiao Guang Sun, Pengfei Cao, Andrew Westover

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

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Abstract

The development of a solid electrolyte that can impede dendrite growth while still maintaining an appropriate level of conductivity is essential for improving performance of solid-state Li-ion battery. In this paper, we report the synthesis of single Li-ion conducting hairy nanoparticle (NP) materials that improved the cycling stability of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-doped poly(ethylene oxide) (PEO) solid electrolyte without significant reduction in conductivity. To unveil mechanisms leading to improved cycling stability, several characterization techniques including broadband dielectric spectroscopy, differential scanning calorimetry, small angle X-ray scattering, transmission electron microscopy, and shear rheology were used to study properties of polymer composites (PC) with added hairy NPs. It was found that hairy NPs influenced the Li/electrolyte interface and improved mechanical properties of bulk composites, all of which contributed to homogenous Li plating and stripping. The improved performance has been found in composites with concentrations of 4.8 and 9.1 weight % of added hairy NPs, which enabled Li cycling stability at 0.2 mA cm^-2 critical current density (>300 h) that was otherwise not possible in either PEO-LiTFSI alone or PEO-LiTFSI composites containing a polymer identical to that attached to hairy NPs. Based on the discovered ability of hairy NP to influence bulk and interfacial properties of solid electrolyte, their use as additives is expected to be equally effective in reducing dendrite formation in other electrolytes relevant for the design of solid-state battery.

Original language	English
Pages (from-to)	8042-8052
Number of pages	11
Journal	ACS Applied Energy Materials
Volume	6
Issue number	15
DOIs	https://doi.org/10.1021/acsaem.3c01106
State	Published - Aug 14 2023

Funding

This research is sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL), managed by UT-Battelle, LLC for the U.S. Department of Energy under contract no. DE-AC05-00OR22725. X.C.C. (transport number analysis, TEM) and R.L.S. (impedance data analysis) were supported by the Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research Program. X.G.S. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division This research used the resources of the Center for Nanophase Materials Sciences (CNMS) under the CNMS user program and Spallation Neutron Source (SNS), which are DOE Office of Science User Facilities. We wish to express our gratitude to Dr. Wim Brass for his valuable insights and constructive discussions on our findings.

Keywords

cycling stability
dendrites
hairy nanoparticles
single ion conducting polymers
solid state battery

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsaem.3c01106

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title = "Single Ion Conducting Hairy Nanoparticle Additive to Improve Cycling Stability of Solid Polymer Electrolytes",

abstract = "The development of a solid electrolyte that can impede dendrite growth while still maintaining an appropriate level of conductivity is essential for improving performance of solid-state Li-ion battery. In this paper, we report the synthesis of single Li-ion conducting hairy nanoparticle (NP) materials that improved the cycling stability of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-doped poly(ethylene oxide) (PEO) solid electrolyte without significant reduction in conductivity. To unveil mechanisms leading to improved cycling stability, several characterization techniques including broadband dielectric spectroscopy, differential scanning calorimetry, small angle X-ray scattering, transmission electron microscopy, and shear rheology were used to study properties of polymer composites (PC) with added hairy NPs. It was found that hairy NPs influenced the Li/electrolyte interface and improved mechanical properties of bulk composites, all of which contributed to homogenous Li plating and stripping. The improved performance has been found in composites with concentrations of 4.8 and 9.1 weight % of added hairy NPs, which enabled Li cycling stability at 0.2 mA cm-2 critical current density (>300 h) that was otherwise not possible in either PEO-LiTFSI alone or PEO-LiTFSI composites containing a polymer identical to that attached to hairy NPs. Based on the discovered ability of hairy NP to influence bulk and interfacial properties of solid electrolyte, their use as additives is expected to be equally effective in reducing dendrite formation in other electrolytes relevant for the design of solid-state battery.",

keywords = "cycling stability, dendrites, hairy nanoparticles, single ion conducting polymers, solid state battery",

author = "Vera Bocharova and Chen, {Xi Chelsea} and Jeong, {Seung Pyo} and Zhengping Zhou and Sacci, {Robert L.} and Keum, {Jong K.} and Catalin Gainaru and Rahman, {Md Anisur} and Ritu Sahori and Sun, {Xiao Guang} and Pengfei Cao and Andrew Westover",

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doi = "10.1021/acsaem.3c01106",

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AU - Bocharova, Vera

AU - Chen, Xi Chelsea

AU - Jeong, Seung Pyo

AU - Zhou, Zhengping

AU - Sacci, Robert L.

AU - Keum, Jong K.

AU - Gainaru, Catalin

AU - Rahman, Md Anisur

AU - Sahori, Ritu

AU - Sun, Xiao Guang

AU - Cao, Pengfei

AU - Westover, Andrew

PY - 2023/8/14

Y1 - 2023/8/14

N2 - The development of a solid electrolyte that can impede dendrite growth while still maintaining an appropriate level of conductivity is essential for improving performance of solid-state Li-ion battery. In this paper, we report the synthesis of single Li-ion conducting hairy nanoparticle (NP) materials that improved the cycling stability of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-doped poly(ethylene oxide) (PEO) solid electrolyte without significant reduction in conductivity. To unveil mechanisms leading to improved cycling stability, several characterization techniques including broadband dielectric spectroscopy, differential scanning calorimetry, small angle X-ray scattering, transmission electron microscopy, and shear rheology were used to study properties of polymer composites (PC) with added hairy NPs. It was found that hairy NPs influenced the Li/electrolyte interface and improved mechanical properties of bulk composites, all of which contributed to homogenous Li plating and stripping. The improved performance has been found in composites with concentrations of 4.8 and 9.1 weight % of added hairy NPs, which enabled Li cycling stability at 0.2 mA cm-2 critical current density (>300 h) that was otherwise not possible in either PEO-LiTFSI alone or PEO-LiTFSI composites containing a polymer identical to that attached to hairy NPs. Based on the discovered ability of hairy NP to influence bulk and interfacial properties of solid electrolyte, their use as additives is expected to be equally effective in reducing dendrite formation in other electrolytes relevant for the design of solid-state battery.

AB - The development of a solid electrolyte that can impede dendrite growth while still maintaining an appropriate level of conductivity is essential for improving performance of solid-state Li-ion battery. In this paper, we report the synthesis of single Li-ion conducting hairy nanoparticle (NP) materials that improved the cycling stability of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-doped poly(ethylene oxide) (PEO) solid electrolyte without significant reduction in conductivity. To unveil mechanisms leading to improved cycling stability, several characterization techniques including broadband dielectric spectroscopy, differential scanning calorimetry, small angle X-ray scattering, transmission electron microscopy, and shear rheology were used to study properties of polymer composites (PC) with added hairy NPs. It was found that hairy NPs influenced the Li/electrolyte interface and improved mechanical properties of bulk composites, all of which contributed to homogenous Li plating and stripping. The improved performance has been found in composites with concentrations of 4.8 and 9.1 weight % of added hairy NPs, which enabled Li cycling stability at 0.2 mA cm-2 critical current density (>300 h) that was otherwise not possible in either PEO-LiTFSI alone or PEO-LiTFSI composites containing a polymer identical to that attached to hairy NPs. Based on the discovered ability of hairy NP to influence bulk and interfacial properties of solid electrolyte, their use as additives is expected to be equally effective in reducing dendrite formation in other electrolytes relevant for the design of solid-state battery.

KW - cycling stability

KW - dendrites

KW - hairy nanoparticles

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JF - ACS Applied Energy Materials

IS - 15

ER -

Single Ion Conducting Hairy Nanoparticle Additive to Improve Cycling Stability of Solid Polymer Electrolytes

Abstract

Funding

Keywords

UN SDGs

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