Title: Single-Ion Conducting Polymer Nanoparticles as Functional Fillers for Solid Electrolytes in Lithium Metal Batteries

Abstract

Composite solid electrolytes including inorganic nanoparticles or nanofibers which improve the performance of polymer electrolytes due to their superior mechanical, ionic conductivity, or lithium transference number are actively being researched for applications in lithium metal batteries. However, inorganic nanoparticles present limitations such as tedious surface functionalization and agglomeration issues and poor homogeneity at high concentrations in polymer matrixes. In this work, we report on polymer nanoparticles with a lithium sulfonamide surface functionality (LiPNP) for application as electrolytes in lithium metal batteries. The particles are prepared by semibatch emulsion polymerization, an easily up-scalable technique. LiPNPs are used to prepare two different families of particle-reinforced solid electrolytes. When mixed with poly(ethylene oxide) and lithium bis(trifluoromethane)sulfonimide (LiTFSI/PEO), the particles invoke a significant stiffening effect (E' > 10⁶ Pa vs 10⁵ Pa at 80 °C) while the membranes retain high ionic conductivity (σ = 6.6 × 10^–4 S cm^–1). Preliminary testing in LiFePO₄ lithium metal cells showed promising performance of the PEO nanocomposite electrolytes. By mixing the particles with propylene carbonate without any additional salt, we obtain true single-ion conducting gel electrolytes, as the lithium sulfonamide surface functionalities are the only sources of lithium ions in the system. The gel electrolytes are mechanically robustmore » (up to G' = 10⁶ Pa) and show ionic conductivity up to 10^–4 S cm^–1. Finally, the PC nanocomposite electrolytes were tested in symmetrical lithium cells. Our findings suggest that all-polymer nanoparticles could represent a new building block material for solid-state lithium metal battery applications.« less

Authors:

Porcarelli, Luca  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-1624-382X"

Sutton, Preston ^[2]; Bocharova, Vera  ^[3];

• Search DOE PAGES for author "Bocharova, Vera"
• Search DOE PAGES for ORCID "0000-0003-4270-3866"

Aguirresarobe, Robert H. ^[4]; Zhu, Haijin ^[2]; Goujon, Nicolas  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-0555-2846"

Leiza, Jose R. ^[4]; Sokolov, Alexei  ^[5];

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• Search DOE PAGES for ORCID "0000-0002-8187-9445"

Forsyth, Maria  ^[6];

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• Search DOE PAGES for ORCID "0000-0002-4273-8105"

Mecerreyes, David  ^[7]

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• Search DOE PAGES for ORCID "0000-0002-0788-7156"

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1. POLYMAT University of the Basque Country UPV/EHU, Joxe Mari Korta Center, Avenida Tolosa 72, 20018, Donostia−San Sebastian, Spain, ARC Centre of Excellence for Electromaterials Science and Institute for Frontier Materials, Deakin University, Melbourne, 3125 Australia
2. ARC Centre of Excellence for Electromaterials Science and Institute for Frontier Materials, Deakin University, Melbourne, 3125 Australia
3. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
4. POLYMAT University of the Basque Country UPV/EHU, Joxe Mari Korta Center, Avenida Tolosa 72, 20018, Donostia−San Sebastian, Spain
5. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States, Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
6. POLYMAT University of the Basque Country UPV/EHU, Joxe Mari Korta Center, Avenida Tolosa 72, 20018, Donostia−San Sebastian, Spain, ARC Centre of Excellence for Electromaterials Science and Institute for Frontier Materials, Deakin University, Melbourne, 3125 Australia, Ikerbasque, Basque Foundation for Science, Maria Diaz de Haro 3, E−48011 Bilbao, Spain
7. POLYMAT University of the Basque Country UPV/EHU, Joxe Mari Korta Center, Avenida Tolosa 72, 20018, Donostia−San Sebastian, Spain, Ikerbasque, Basque Foundation for Science, Maria Diaz de Haro 3, E−48011 Bilbao, Spain

Publication Date:

Wed Nov 03 00:00:00 EDT 2021

Research Org.:

Univ. of the Basque Country (UPV/EHU), San Sebastian (Spain); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:

USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; European Research Council (ERC); Swiss National Science Foundation (SNSF); Basque Government

OSTI Identifier:

1828799

Alternate Identifier(s):

OSTI ID: 1831414; OSTI ID: 1836412

Grant/Contract Number:  

AC05-00OR22725; 797295; P2FRP2_191846; IT99-16

Resource Type:

Published Article

Journal Name:

ACS Applied Materials and Interfaces

Additional Journal Information:

Journal Name: ACS Applied Materials and Interfaces Journal Volume: 13 Journal Issue: 45; Journal ID: ISSN 1944-8244

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE; single-ion; nanoparticle; lithium; electrolyte; gel; solid-state; battery