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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2024-12-01
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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 |
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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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