Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes
Environmental impacts and resource availability are significant concerns for the future of lithium-ion batteries. This study focuses on developing novel fluorine-free electrolytes compatible with aqueous-processed cobalt-free cathode materials. The new electrolyte contains lithium 1,1,2,3,3-pentacya...
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MDPI AG
2024-10-01
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| Online Access: | https://www.mdpi.com/1420-3049/29/19/4698 |
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| author | Claudia Limachi Klaudia Rogala Marek Broszkiewicz Marta Cabello Leszek Niedzicki Michel Armand Władysław Wieczorek |
| author_facet | Claudia Limachi Klaudia Rogala Marek Broszkiewicz Marta Cabello Leszek Niedzicki Michel Armand Władysław Wieczorek |
| author_sort | Claudia Limachi |
| collection | DOAJ |
| description | Environmental impacts and resource availability are significant concerns for the future of lithium-ion batteries. This study focuses on developing novel fluorine-free electrolytes compatible with aqueous-processed cobalt-free cathode materials. The new electrolyte contains lithium 1,1,2,3,3-pentacyanopropenide (LiPCP) salt. After screening various organic carbonates, a mixture of 30:70 wt.% ethylene carbonate and dimethyl carbonate was chosen as the solvent. The optimal salt concentration, yielding the highest conductivity of 9.6 mS·cm<sup>−1</sup> at 20 °C, was 0.8 mol·kg<sup>−1</sup>. Vinylene carbonate was selected as a SEI-stabilizing additive, and the electrolyte demonstrated stability up to 4.4 V vs. Li+/Li. LiFePO<sub>4</sub> and LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> were identified as suitable cobalt-free cathode materials. They were processed using sodium carboxymethyl cellulose as a binder and water as the solvent. Performance testing of various cathode compositions was conducted using cyclic voltammetry and galvanostatic cycling with the LiPCP-based electrolyte and a standard LiPF6-based one. The optimized cathode compositions, with an 87:10:3 ratio of active material to conductive additive to binder, showed good compatibility and performance with the new electrolyte. Aqueous-processed LiFePO<sub>4</sub> and LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> achieved capacities of 160 mAh·g<sup>−1</sup> and 70 mAh·g<sup>−1</sup> at C/10 after 40 cycles, respectively. These findings represent the first stage of investigating LiPCP for the development of greener and more sustainable lithium-ion batteries. |
| format | Article |
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| institution | OA Journals |
| issn | 1420-3049 |
| language | English |
| publishDate | 2024-10-01 |
| publisher | MDPI AG |
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| series | Molecules |
| spelling | doaj-art-92a4f7520c6a409d8fbbe140a5fa2b2a2025-08-20T02:16:55ZengMDPI AGMolecules1420-30492024-10-012919469810.3390/molecules29194698Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate CathodesClaudia Limachi0Klaudia Rogala1Marek Broszkiewicz2Marta Cabello3Leszek Niedzicki4Michel Armand5Władysław Wieczorek6Faculty of Chemistry, Warsaw University of Technology, 00-664 Warsaw, PolandFaculty of Chemistry, Warsaw University of Technology, 00-664 Warsaw, PolandFaculty of Chemistry, Warsaw University of Technology, 00-664 Warsaw, PolandCentre for Cooperative Research on Alternative Energies (CIC energiGUNE), Basque Research and Technology Alliance (BRTA), Alava Technology Park, Albert Einstein 48, 01510 Vitoria-Gasteiz, SpainFaculty of Chemistry, Warsaw University of Technology, 00-664 Warsaw, PolandCentre for Cooperative Research on Alternative Energies (CIC energiGUNE), Basque Research and Technology Alliance (BRTA), Alava Technology Park, Albert Einstein 48, 01510 Vitoria-Gasteiz, SpainFaculty of Chemistry, Warsaw University of Technology, 00-664 Warsaw, PolandEnvironmental impacts and resource availability are significant concerns for the future of lithium-ion batteries. This study focuses on developing novel fluorine-free electrolytes compatible with aqueous-processed cobalt-free cathode materials. The new electrolyte contains lithium 1,1,2,3,3-pentacyanopropenide (LiPCP) salt. After screening various organic carbonates, a mixture of 30:70 wt.% ethylene carbonate and dimethyl carbonate was chosen as the solvent. The optimal salt concentration, yielding the highest conductivity of 9.6 mS·cm<sup>−1</sup> at 20 °C, was 0.8 mol·kg<sup>−1</sup>. Vinylene carbonate was selected as a SEI-stabilizing additive, and the electrolyte demonstrated stability up to 4.4 V vs. Li+/Li. LiFePO<sub>4</sub> and LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> were identified as suitable cobalt-free cathode materials. They were processed using sodium carboxymethyl cellulose as a binder and water as the solvent. Performance testing of various cathode compositions was conducted using cyclic voltammetry and galvanostatic cycling with the LiPCP-based electrolyte and a standard LiPF6-based one. The optimized cathode compositions, with an 87:10:3 ratio of active material to conductive additive to binder, showed good compatibility and performance with the new electrolyte. Aqueous-processed LiFePO<sub>4</sub> and LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> achieved capacities of 160 mAh·g<sup>−1</sup> and 70 mAh·g<sup>−1</sup> at C/10 after 40 cycles, respectively. These findings represent the first stage of investigating LiPCP for the development of greener and more sustainable lithium-ion batteries.https://www.mdpi.com/1420-3049/29/19/4698fluorine-free lithium saltslithium-ion batteriesgreen chemistrysustainabilityaqueous electrodesaqueous binders |
| spellingShingle | Claudia Limachi Klaudia Rogala Marek Broszkiewicz Marta Cabello Leszek Niedzicki Michel Armand Władysław Wieczorek Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes Molecules fluorine-free lithium salts lithium-ion batteries green chemistry sustainability aqueous electrodes aqueous binders |
| title | Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes |
| title_full | Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes |
| title_fullStr | Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes |
| title_full_unstemmed | Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes |
| title_short | Development of Fluorine-Free Electrolytes for Aqueous-Processed Olivine-Type Phosphate Cathodes |
| title_sort | development of fluorine free electrolytes for aqueous processed olivine type phosphate cathodes |
| topic | fluorine-free lithium salts lithium-ion batteries green chemistry sustainability aqueous electrodes aqueous binders |
| url | https://www.mdpi.com/1420-3049/29/19/4698 |
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