A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders

Lithium-ion batteries are a promising technology to promote the phase-out of fossil fuel vehicles. Increasing efforts are focused on improving their energy density and safety by replacing current materials with more efficient and safer alternatives. In this context, binary composites of organic ioni...

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Main Authors: Daniela M. Josepetti, Maria Forsyth, Patrick C. Howlett, Hiroyuki Ueda
Format: Article
Language:English
Published: MDPI AG 2024-12-01
Series:Batteries
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Online Access:https://www.mdpi.com/2313-0105/11/1/3
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author Daniela M. Josepetti
Maria Forsyth
Patrick C. Howlett
Hiroyuki Ueda
author_facet Daniela M. Josepetti
Maria Forsyth
Patrick C. Howlett
Hiroyuki Ueda
author_sort Daniela M. Josepetti
collection DOAJ
description Lithium-ion batteries are a promising technology to promote the phase-out of fossil fuel vehicles. Increasing efforts are focused on improving their energy density and safety by replacing current materials with more efficient and safer alternatives. In this context, binary composites of organic ionic plastic crystals (OIPCs) and lithium salts show promise due to their impressive mechanical properties and ionic conductivity. Taking advantage of this, the present paper substitutes the commercial non-electrochemically active binder with an OIPC component, <i>N</i>-ethyl-<i>N</i>-methylpyrrolidinium bis(fluorosulfonyl)imide ([C<sub>2</sub>mpyr][FSI]), in combination with LiFSI. Slurry-formulation experiments revealed that varying the new binder’s composition allows the production of diverse LiFePO<sub>4</sub> (LFP) cathodes via the conventional fabrication process. Large amounts of OIPC−lithium salt mixtures in the composition yielded thick electrodes with expected nominal areal capacities of up to 3.74 mAh/cm<sup>2</sup>, where the balanced composition with a reduced Li<sup>+</sup> concentration can demonstrate >1.5 mAh/cm<sup>2</sup> at 0.1C. Lowering the amount of these ion-conductive binders enabled LFP cathodes to perform effectively under fast cycling conditions at a C-rate as high as 2C. Preliminary battery tests with a limited Li<sup>+</sup> source demonstrated the feasibility of full-cell operation without using the lithium-metal anode. This work paves the way for developing advanced rechargeable batteries using OIPC-based ion-conductive binders for a wide range of applications.
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spelling doaj-art-7eed739a7de44d98aad8364ddf04ceaf2025-01-24T13:22:21ZengMDPI AGBatteries2313-01052024-12-01111310.3390/batteries11010003A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive BindersDaniela M. Josepetti0Maria Forsyth1Patrick C. Howlett2Hiroyuki Ueda3Institute for Frontier Materials (IFM), Deakin University, 221 Burwood Highway, Burwood 3125, AustraliaInstitute for Frontier Materials (IFM), Deakin University, 221 Burwood Highway, Burwood 3125, AustraliaInstitute for Frontier Materials (IFM), Deakin University, 221 Burwood Highway, Burwood 3125, AustraliaInstitute for Frontier Materials (IFM), Deakin University, 221 Burwood Highway, Burwood 3125, AustraliaLithium-ion batteries are a promising technology to promote the phase-out of fossil fuel vehicles. Increasing efforts are focused on improving their energy density and safety by replacing current materials with more efficient and safer alternatives. In this context, binary composites of organic ionic plastic crystals (OIPCs) and lithium salts show promise due to their impressive mechanical properties and ionic conductivity. Taking advantage of this, the present paper substitutes the commercial non-electrochemically active binder with an OIPC component, <i>N</i>-ethyl-<i>N</i>-methylpyrrolidinium bis(fluorosulfonyl)imide ([C<sub>2</sub>mpyr][FSI]), in combination with LiFSI. Slurry-formulation experiments revealed that varying the new binder’s composition allows the production of diverse LiFePO<sub>4</sub> (LFP) cathodes via the conventional fabrication process. Large amounts of OIPC−lithium salt mixtures in the composition yielded thick electrodes with expected nominal areal capacities of up to 3.74 mAh/cm<sup>2</sup>, where the balanced composition with a reduced Li<sup>+</sup> concentration can demonstrate >1.5 mAh/cm<sup>2</sup> at 0.1C. Lowering the amount of these ion-conductive binders enabled LFP cathodes to perform effectively under fast cycling conditions at a C-rate as high as 2C. Preliminary battery tests with a limited Li<sup>+</sup> source demonstrated the feasibility of full-cell operation without using the lithium-metal anode. This work paves the way for developing advanced rechargeable batteries using OIPC-based ion-conductive binders for a wide range of applications.https://www.mdpi.com/2313-0105/11/1/3polymer-binder-free cathodesion-conductive bindersorganic ionic plastic crystalsionic liquidslithium metal batteriesrechargeable batteries
spellingShingle Daniela M. Josepetti
Maria Forsyth
Patrick C. Howlett
Hiroyuki Ueda
A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders
Batteries
polymer-binder-free cathodes
ion-conductive binders
organic ionic plastic crystals
ionic liquids
lithium metal batteries
rechargeable batteries
title A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders
title_full A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders
title_fullStr A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders
title_full_unstemmed A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders
title_short A Polymer-Binder-Free Approach to Creating Functional LiFePO<sub>4</sub> Cathodes by Organic Ionic Plastic Crystal-Derived Ion-Conductive Binders
title_sort polymer binder free approach to creating functional lifepo sub 4 sub cathodes by organic ionic plastic crystal derived ion conductive binders
topic polymer-binder-free cathodes
ion-conductive binders
organic ionic plastic crystals
ionic liquids
lithium metal batteries
rechargeable batteries
url https://www.mdpi.com/2313-0105/11/1/3
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