ABSTRACT
The rational design of highly active and low-cost electrode material is very promising for energy storage applications. The development of supercapacitors with high energy/power density is an imperative and challenging research objective. Herein, we report a highly facile synthesis approach for developing unique nano-porous hybrid NiCuMn oxyhydroxide architecture with remarkable electrochemical energy storage characteristics. The process involves dealloying of Ni15Cu15Mn70alloy in an oxygen rich environment, resulting in a uniform 3-dimensional flower like morphology. The dealloyed electrode demonstrates ultra-high specific capacitance of 4110 F cm-3at a high current density of 20 mA cm-2. A symmetric device exhibits a high volumetric capacitance of 365 F cm-3at a current density of 10 mA cm-2with a large potential window of 1.7 V. Even at very high-power density of 850 W l-1, the device exhibits a high energy density of 146 Wh l-1along with remarkable cyclic stability of 95.4% after 10 000 cycles. The superior performance of nano-porous hybrid NiCuMn oxyhydroxide architecture was attributed to its unique microstructure that provides high surface area, and marginal internal resistance ensuring rapid charge transport.
ABSTRACT
High-performance energy storage devices (HPEDs) play a critical role in the realization of clean energy and thus enable the overarching pursuit of nonpolluting, green technologies. Supercapacitors are one class of such lucrative HPEDs; however, a serious limiting factor of supercapacitor technology is its sub-par energy density. This report presents hitherto unchartered pathway of physical deformation, chemical dealloying, and microstructure engineering to produce ultrahigh-capacitance, energy-dense NiMn alloy electrodes. The activated electrode delivered an ultrahigh specific-capacitance of 2700 F/cm3 at 0.5 A/cm3. The symmetric device showcased an excellent energy density of 96.94 Wh/L and a remarkable cycle life of 95% retention after 10,000 cycles. Transmission electron microscopy and atom probe tomography studies revealed the evolution of a unique hierarchical microstructure comprising fine Ni/NiMnO3 nanoligaments within MnO2-rich nanoflakes. Theoretical analysis using density functional theory showed semimetallic nature of the nanoscaled oxygen-vacancy-rich NiMnO3 structure, highlighting enhanced carrier concentration and electronic conductivity of the active region. Furthermore, the geometrical model of NiMnO3 crystals revealed relatively large voids, likely providing channels for the ion intercalation/de-intercalation. The current processing approach is highly adaptable and can be applied to a wide range of material systems for designing highly efficient electrodes for energy-storage devices.
