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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Main Authors: Claudia Limachi, Klaudia Rogala, Marek Broszkiewicz, Marta Cabello, Leszek Niedzicki, Michel Armand, Władysław Wieczorek
Format: Article
Language:English
Published: MDPI AG 2024-10-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/29/19/4698
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Summary: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.
ISSN:1420-3049