Temperature-Controlled Synthesis of Li- and Mn-Rich Li1.2Mn0.54Ni0.13Co0.13O2 Hollow Nano/Sub-Microsphere Electrodes for High-Performance Lithium-Ion Battery

Srinivasan Alagar; Chelladurai Karuppiah; Rajesh Madhuvilakku; Shakkthivel Piraman; Chun-Chen Yang

doi:10.1021/acsomega.9b02766

Temperature-Controlled Synthesis of Li- and Mn-Rich Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ Hollow Nano/Sub-Microsphere Electrodes for High-Performance Lithium-Ion Battery

ACS Omega. 2019 Nov 21;4(23):20285-20296. doi: 10.1021/acsomega.9b02766. eCollection 2019 Dec 3.

Authors

Srinivasan Alagar¹, Chelladurai Karuppiah², Rajesh Madhuvilakku¹, Shakkthivel Piraman¹, Chun-Chen Yang²

Affiliations

¹ Sustainable Energy and Smart Materials Research Lab, Department of Nanoscience and Technology, Science Campus, Alagappa University, Karaikudi 630002, Tamil Nadu, India.
² Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, ROC.

Abstract

The calcination temperature plays a significant role in the structural, textural, and energy-storage performance of metal oxide nanomaterials in Li-ion battery application. Here, we report the formation of well-crystallized homogeneously dispersed Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ hollow nano/sub-microsphere architectures through a simple cost-effective coprecipitation and chemical mixing route without surface modification for improving the efficiency of energy storage devices. The synthesized Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ hollow nano/sub-microsphere cathode materials are calcined at 800, 900, 950, and 1000 °C. Among them, Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ calcined at 950 °C exhibits a high discharge capacity (277 mAh g^-1 at 0.1C rate) and excellent capacity retention (88%) after 50 cycles and also delivers an excellent discharge capacity of >172 mAh g^-1 at 5C rate. Good electrochemical performance of Li_1.2Mn_0.54Ni_0.13Co_0.13O₂-950 is directly related to the optimized size of its primary particles (85 nm) (which constitute the spherical secondary particle, ∼720 nm) and homogeneous cation mixing. Higher calcination temperature (≥950 °C) leads to an increase of the primary particle size, poor cycling stability, and inferior rate capacity of Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ due to smashing of quasi-hollow spheres upon repeated lithium ion intercalations/deintercalations. Therefore, Li_1.2Mn_0.54Ni_0.13Co_0.13O₂-950 is a promising electrode for the next-generation high-voltage and high-capacity Li-ion battery application.