Single-ion conducting polymer nanoparticles as functional fillers for solid electrolytes in lithium metal batteries

TY - JOUR

T1 - Single-ion conducting polymer nanoparticles as functional fillers for solid electrolytes in lithium metal batteries

AU - Porcarelli, Luca

AU - Sutton, Preston

AU - Bocharova, Vera

AU - Aguirresarobe, Robert H.

AU - Zhu, Haijin

AU - Goujon, Nicolas

AU - Leiza, Jose R.

AU - Sokolov, Alexei

AU - Forsyth, Maria

AU - Mecerreyes, David

N1 - Publisher Copyright: ©

PY - 2021/11/17

Y1 - 2021/11/17

N2 - 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 robust (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.

AB - 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 robust (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.

KW - battery

KW - electrolyte

KW - gel

KW - lithium

KW - nanoparticle

KW - single-ion

KW - solid-state

UR - http://www.scopus.com/inward/record.url?scp=85119453706&partnerID=8YFLogxK

U2 - 10.1021/acsami.1c15771

DO - 10.1021/acsami.1c15771

M3 - 文章

C2 - 34730327

AN - SCOPUS:85119453706

SN - 1944-8244

VL - 13

SP - 54354

EP - 54362

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

IS - 45

ER -