The electrochemical performance of cells with a Li 1.03 (Ni 0.5 Co 0.2 Mn 0.3 ) 0.97 O 2 (NCM523) positive electrode and a blended silicongraphite (Si-Gr) negative electrode are investigated using various electrolyte compositions and voltage cycling windows. Voltage profiles of the blended Si-Gr electrode show a superposition of graphite potential plateaus on a sloped Si profile with a large potential hysteresis. The effect of this hysteresis is seen in the cell impedance versus voltage data, which are distinctly different for the charge and discharge cycles. We confirm that the addition of compounds, such as vinylene carbonate (VC) and fluoroethylene carbonate (FEC) to the baseline 1.2 M LiPF 6 in ethylene carbonate (EC): ethyl methyl carbonate (EMC) (3:7 w/w) electrolyte, improves cell capacity retention with higher retention seen at higher additive contents. We show that reducing the lower cutoff voltage (LCV) of full cells to 2.5 V increases the Si-Gr electrode potential to 1.12 V vs. Li/Li + ; this relatively-high delithiation potential correlates with the lower capacity retention displayed by the cell. Furthermore, we show that raising the upper cutoff voltage (UCV) can increase cell energy density without significantly altering capacity retention over 100 charge-discharge cycles. The development of new high-energy electrochemical couples is important to reducing the overall cost and weight per kWh of Li-ion batteries. Silicon and silicon-containing blended electrodes have been a focus of much recent research as an alternative to the commercial graphite-based negative electrode because of the substantially higher theoretical capacity of silicon (3579 mAh g −1 , Li 15 Si 4 ) compared to that of graphite (372 mAh g −1 , LiC 6 ); the higher capacity enables reduction of the negative electrode weight thereby increasing energy density of the cell. However, concerns including electrode integrity and durability related to the substantial volume expansion/contraction (∼300%) of silicon during lithiation/delithiation reactions have hampered the use of silicon as a direct substitute for graphite.Several strategies to overcome the durability problems target design of the composite electrode and its components. For example, purposely-designed silicon particle morphologies 1-3 and the use of graphene 4,5 are reported to improve the cycle life of electrodes in cells with a Li-metal counter electrode (half-cells). The choice of binders also greatly influences electrode coherence; 6-10 for example lithiated polyacrylic acid (LiPAA) has been shown to increase cycle life compared to e.g. polyvinylidene fluoride (PVDF). 6,8,10 Direct incorporation and mixing of silicon particles into standard graphite slurries also provides a means of incrementally improving electrode capacity, while retaining the higher durability of graphite electrodes.
11-13In addition to variations in the electrode constitution, alternative electrolytes are being studied to improve cell cycling stability by tuning the electrochemical interfaces. The use ...