Insights on the cycling behavior of a highly-prelithiated silicon–graphite electrode in lithium-ion cells

MTF Rodrigues, JA Gilbert, K Kalaga… - Journal of Physics …, 2020 - iopscience.iop.org
Journal of Physics: Energy, 2020iopscience.iop.org
Nanosized silicon materials are being developed for use in the anodes of high-energy
lithium-ion batteries. However, the high surface areas of these materials increase the rate of
parasitic reactions in the electrode, which consume cyclable Li+ and degrade battery
performance. Prelithiation offers a realistic strategy to compensate for this reactivity, by
injecting additional charge into the cell to counterbalance the Li+ loss. Interestingly, the
benefits offered by prelithiation extend beyond its more obvious purpose. Here, by using a …
Abstract
Nanosized silicon materials are being developed for use in the anodes of high-energy lithium-ion batteries. However, the high surface areas of these materials increase the rate of parasitic reactions in the electrode, which consume cyclable Li+ and degrade battery performance. Prelithiation offers a realistic strategy to compensate for this reactivity, by injecting additional charge into the cell to counterbalance the Li+ loss. Interestingly, the benefits offered by prelithiation extend beyond its more obvious purpose. Here, by using a reference electrode in NMC532//Si–Gr cells, we show how prelithiation alters the cycling potentials experienced by the Si-containing anode and how that translates into gains in cycle life. The rate of consumption of the prelithiated charge is lower than that expected from the behavior of non-prelithiated cells. Curiously, the Si particles become partially unresponsive during the C/3 cycling apparently because of kinetic constraints. Electrochemical studies on harvested electrodes in half-cells show that capacities are intact after the long-term cycling and that most of the lithium reservoir is still present in the anode. We conclude that the high capacity retention displayed by the prelithiated cells mainly results from a higher participation of graphite particles during the extended electrochemical cycling.
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