Summary
In this paper, a systematic method has been developed to produce highly flexible and robust graphene/LiMn2O4 (G/LMO) and graphene/LiCr0.05Mn1.95O4 (G/LCMO) free‐standing composite cathode electrodes with increased specific capacity and improved electrochemical capability. Spinel LMO nanorods are synthesized by calcination method followed by a hydrothermal reaction technique. As‐synthesized nanorods were then embedded in a graphene layer which will in turn serve as a self‐standing binder‐free cathode electrode. Spinel LMO and LCMO nanorods with a length of 600 nm and width of 50 nm were then homogenously entrapped and distributed within the layers of conductive graphene structure. This hybrid structure will help to eliminate the use of heavy metal current collectors and electrically resistant binders or even conductive additives. A discharge capacity of 114.5 mAh g−1 is obtained after first cycle and %72 capacity retention is obtained after 250 cycles from G/LCMO freestanding samples. The enhancement in the electrochemical properties is due to the unique freestanding structure of the cathode electrodes.
The cathode electrodes in commercial Li-ion cells are usually coated on aluminum foils, while the anode part is coated on copper current collector. However, these metallic foils of the electrodes are relatively heavy counterparts when compared with the total cell weight. To overcome this issue, we comparatively studied LiNi 1/3 Mn 1/3 Co 1/3 O 2 (NMC); NMC/graphene positive electrodes reinforced with graphene were produced in the form of freestanding electrodes by a facile sol-gel and vacuum filtration method. To confirm our results obtained with the half-cells, graphite@NMC@graphene full-cells were also produced and a specific capacity of 220 mAh g −1 after 250 cycles. Extraordinary electrochemical cycling, high conductivity, and enhanced rate properties are obtained by anchoring the NMC particles between the graphene layers. The results have also indicated that the freestanding graphene-based electrodes could be a useful tool for high-capacity lithium-ion batteries.
Different polymorphs of MnO2 (α-, β-, and γ-) were produced by microwave hydrothermal synthesis, and graphene oxide (GO) nanosheets were prepared by oxidation of graphite using a modified Hummers’ method. Freestanding graphene/MnO2 cathodes were manufactured through a vacuum filtration process. The structure of the graphene/MnO2 nanocomposites was characterized using X-ray diffraction (XRD) and Raman spectroscopy. The surface and cross-sectional morphologies of freestanding cathodes were investigated by scanning electron microcopy (SEM). The charge–discharge profile of the cathodes was tested between 1.5 V and 4.5 V at a constant current of 0.1 mA cm−2 using CR2016 coin cells. The initial specific capacity of graphene/α-, β-, and γ-MnO2 freestanding cathodes was found to be 321 mAhg−1, 198 mAhg−1, and 251 mAhg−1, respectively. Finally, the graphene/α-MnO2 cathode displayed the best cycling performance due to the low charge transfer resistance and higher electrochemical reaction behavior. Graphene/α-MnO2 freestanding cathodes exhibited a specific capacity of 229 mAhg−1 after 200 cycles with 72% capacity retention.
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