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Molecules 2017, 22, 403 3 of 21 (formation cycles) of the LIB cell and is essential for safety and performance due to its protection of the electrolyte from further reductive decomposition at the anode surface [79–81]. Figure 1. Structures of six of the most important linear and cyclic organic carbonates and the conducting salt lithium hexafluorophosphate for the electrolyte system in lithium ion batteries [60,61]. 3. Aging of Lithium Ion Battery Electrolytes For a better customer acceptance of LIBs, their capacity loss and therefore the reduction of their operating lifetime has to be minimized. The lifetime is limited by several aging mechanisms inside the cell and its components [14,15,30,82,83]. As stated in Section 2, the electrolyte is a mixture since it has to meet several requirements. Unfortunately, the salt lithium hexafluorophosphate is neither chemically nor thermally stable. A thermal equilibrium between LiPF6 and LiF/PF5 (Equation (1)) exists and PF5 as a strong Lewis acid then further reacts with traces of water (present due to the high hygroscopicity of PF6) to POF3 (Equation (2)). With additional water, POF3 is hydrolyzed to difluorophosphoric acid (Equation (3)), monofluorophosphoric acid (Equation (4)) and finally to phosphoric acid (Equation (5)) [35,84–88]. LiPF6 LiF + PF5 (1) PF5 + H2O2HF + POF3 (2) POF3 + H2OHF + HPO2F2 (3) HPO2F2 + H2OHF + H2PO3F (4) H2PO3F + H2OHF + H3PO4 (5) PF5 can also initiate the transesterification of EMC to DMC and DEC (Figure 2a) [89]. Furthermore, the described hydrolysis products can react with the organic carbonate solvent to foster numerous organophosphate-based and organic fluorophosphate-based aging products (Figure 2c,d) [43]. Oligomeric carbonate-based decomposition products are formed by the electrochemically induced ring opening of EC and reaction with the linear carbonates (Figure 2b) [84,90,91]. The exact formation mechanism of the oligomeric carbonate-based compounds is still under discussion.PDF Image | CO2 for Recycling and Sample Preparation of Lithium Ion Battery
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