Reduced Graphene Oxide Sheets Attached Tin Oxalate Dihydrate As a High Capacity Anode for Lithium Ion Rechargeable Batteries

Abstract

Lithium ion batteries have been widely applied as power sources for electronic devices to electric vehicle because of their high energy density, and long cycle life. Commercial graphite is the most commonly used as the anode material for lithium ion batteries. However graphite has its low theoretical capacity (372 mAh g-1). Therefore, to satisfy the growing power requirements, we need to explore alternative materials to replace graphite anode. For these reason, the silicon-based materials, transition metal oxides have been intensively investigated to replace the commercial graphite due to their high capacities, 700 ~ 1000 mAh g-1. Metal oxalate MC2O4 (M : Mn, Fe, Co, Ni, Sn, Cu, Zn) are also interesting because of high capacity. In this study, we synthesize tin oxalate by hydrothermal reaction, of SnCl2ㆍ6H2O (0.001 M), NaC2O4 (0.005 M), distilled water (9 ml), and ethylene glycol (EG, 16 ml) were mixed in a beaker and the mixed solution was stirred at room temperature for 6 h to form transparent solution. This solution was filled in a Teflon-lined autoclave (100ml capacity). This autoclave was sealed and heated at 100 oC - 200 oC for 12 h. After then, the autoclave was cooled to room temperature. The reacted solution were filtered and washed several times with de-ionized water and then dried at 80 oC for 24 h in a convection oven. Also, various contents of rGO were attached by layer by layer method. The obtained powder was analyzed by X-Ray diffraction (XRD, Rigaku, D-max 2000) using CuKα radiation. The XRD data were obtained with 0.03 step size and a 1 s count time. The particle morphologies of the products were analyzed by scanning electron microscopy (SEM, Hitachi, S-4700) and transmission electron microscopy (TEM, Hitachi, H-800). Electrochemical properties were measured in 2032 coin type cell. Electrodes were fabricated from a mixture of the prepared SnC2O4ㆍ2H2O powders (80 wt%), ketjen black (5 wt%), super-P (5 wt%) and polyacrylic acid (10 wt%) in distilled water. The obtained slurry was then applied onto Copper foil and dried in a vacuum oven at 80 oC for 1 h. The electrode was further dried over night at 80 oC under vacuum. The used electrode solution was 1M LiPF6 in a 3 : 7 volume mixture of ethylene carbonate (EC) and dimethyl carbonate (DMC) mixture. The XRD pattern of the products showed single phase SnC2O4ㆍ2H2O and rGO attached both were obtained without impurity. The fabricated cells were charged and discharged in the range of 0 - 3 V applying a constant current of 100 mAg-1 at 25 oC. The bare sample delivered capacity approximately 643 mAh g-1 at initial charge. Also, the delivered capacities increased to 1170, 1220, 1440 mAh g-1 with increasing the amount of rGO (10, 20, 30 wt%). The rate capability demonstrate that the 30 wt% rGO composite SnC2O4ㆍ2H2O / rGO electrode delivered 467 mAh g-1 at 10 C-rate. Figure 1