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Raising the cycling stability of aqueous lithium-ion batteries by eliminating oxygen in the electrolyte


Aqueous lithium-ion batteries may solve the safety problem associated with lithium-ion batteries that use highly toxic and flammable organic solvents, and the poor cycling life associated with commercialized aqueous rechargeable batteries such as lead-acid and nickel-metal hydride systems. But all reported aqueous lithium-ion battery systems have shown poor stability: the capacity retention is typically less than 50% after 100 cycles. Here, the stability of electrode materials in an aqueous electrolyte was extensively analysed. The negative electrodes of aqueous lithium-ion batteries in a discharged state can react with water and oxygen, resulting in capacity fading upon cycling. By eliminating oxygen, adjusting the pH values of the electrolyte and using carbon-coated electrode materials, LiTi2(PO4)3/Li2SO4/LiFePO4 aqueous lithium-ion batteries exhibited excellent stability with capacity retention over 90% after 1,000 cycles when being fully charged/discharged in 10 minutes and 85% after 50 cycles even at a very low current rate of 8 hours for a full charge/discharge offering an energy storage system with high safety, low cost, long cycling life and appropriate energy density.

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Figure 1: The intercalation potential of some electrode materials that could possibly be used for aqueous lithium-ion batteries.
Figure 2: Cyclic voltammograms of LiTi2(PO4)3 at the 1st, 2nd, 3rd, 5th and 10th cycles.
Figure 3: Typical charge/discharge curves of LiTi2(PO4)3 at 4C and 1C charge/discharge rates in the presence/absence of O2.
Figure 4: The typical self-discharge curves of LiTi2(PO4)3 in an aqueous electrolyte at pH 13.
Figure 5: Typical charge/discharge curves of the LiTi2(PO4)3/LiFePO4 aqueous lithium-ion battery.
Figure 6: Cycling life test of the LiTi2(PO4)3/LiFePO4 aqueous lithium-ion battery.

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We acknowledge the support of the National Natural Science Foundation of China (20633040, 20925312), the State Key Basic Research Program of PRC (2007CB209703), and Shanghai Science & Technology Committee (09XD1400300, 08DZ2270500).

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J.L., W.C., P.H. and Y.X. conceived and designed the experiments, analysed and discussed results and commented on the manuscript. J.L. and W.C. performed the experiments and analysed the data. J.L. and Y.X. co-wrote the paper.

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Correspondence to Yong-Yao Xia.

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The authors declare no competing financial interests.

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Luo, JY., Cui, WJ., He, P. et al. Raising the cycling stability of aqueous lithium-ion batteries by eliminating oxygen in the electrolyte. Nature Chem 2, 760–765 (2010).

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