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Strategic Integration of Cobalt-Free Layered-Spinel Cathodes via Solution Combustion Method for High-Performance
Prasanthi Ramesh1, Subramanian Nithiananth2, Kalaivani Raman3
1Futuristic Energy Storage Technology Laboratory (FESTL), Department of Chemistry, SRM Institute of Science and Technology, Kattankulathur, Chennai, Tamil Nadu 603203, India.
ACS Omega
|December 1, 2025
Summary
A novel cobalt-free layered-spinel cathode material (LNMO) was synthesized using sucrose-assisted solution combustion. The LNMO-850 sample showed excellent electrochemical performance, highlighting its potential for advanced battery applications.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Development of cobalt-free cathode materials is crucial for sustainable lithium-ion batteries.
- Layered-spinel structures offer potential for high energy density and stability.
Purpose of the Study:
- To synthesize and characterize a structurally integrated cobalt-free layered-spinel cathode material (Li1.2Ni0.24Mn0.56O2, LNMO).
- To optimize the synthesis conditions, specifically calcination temperature, for enhanced electrochemical performance.
- To evaluate the material's performance at various current densities and temperatures.
Main Methods:
- Sucrose-assisted solution combustion method (SCM) for LNMO synthesis.
- Calcination at different temperatures (650, 750, 850, 950 °C).
- Material characterization using X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), and cyclic voltammetry (CV).
- Electrochemical performance testing at various current densities and temperatures (0-50 °C).
- Postcycling analysis including ex-situ XRD, Raman, and HRSEM.
Main Results:
- The LNMO material comprises both Li-rich layered and spinel phases.
- The sample calcined at 850 °C (LNMO-850) exhibited optimal phase composition and superior electrochemical performance.
- LNMO-850 achieved a maximum specific capacity of 283 mAh g⁻¹ and an energy density of 952 Wh kg⁻¹ at 20 mA g⁻¹.
- At 200 mA g⁻¹, LNMO-850 retained 138 mAh g⁻¹ with 97% Coulombic efficiency after 100 cycles.
- Excellent performance was observed across a temperature range of 0 to 50 °C.
Conclusions:
- The sucrose-assisted solution combustion method is effective for synthesizing cobalt-free layered-spinel cathode materials.
- Calcination at 850 °C yields an optimal phase structure for LNMO, resulting in exceptional electrochemical properties.
- LNMO-850 demonstrates significant potential as a high-performance cathode material for advanced energy storage applications, offering high capacity, energy density, and good cycling stability.
