Insight into the microscopic morphology and electrochemical performance correlation mechanism upon calcination at different temperatures of a novel spherical cobalt-free 0.6Li2MnO3·0.4Li[Fe1/3Ni1/3Mn1/3]O2 cathode

Zhuangzhi Li; Bingshu Guo; Ke Qu; Pei Li; Xinhui Liu; Yifu Jin; Junchen Chen; Zhiyuan Ma; Yun Huang; Mingshan Wang; Rong Huang; Zhenzhong Yang; Xing Li

doi:10.1039/D1SE00312G

Insight into the microscopic morphology and electrochemical performance correlation mechanism upon calcination at different temperatures of a novel spherical cobalt-free 0.6Li₂MnO₃·0.4Li[Fe_1/3Ni_1/3Mn_1/3]O₂ cathode†

Zhuangzhi Li,

^a Bingshu Guo,^a Ke Qu,*^b Pei Li,^a Xinhui Liu,^a Yifu Jin,^a Junchen Chen,^a Zhiyuan Ma,^a Yun Huang,^a Mingshan Wang,

^a Rong Huang,^b Zhenzhong Yang*^b and Xing Li

*^a

Author affiliations

* Corresponding authors

^a School of New Energy and Materials, Southwest Petroleum University, Chengdu, Sichuan 610500, P.R. China
E-mail: lixing198141@yahoo.com
Fax: +86 28 83037409
Tel: +86 28 83037409

^b Key Laboratory of Polar Materials and Devices (MOE), Department of Electronics, East China Normal University, Shanghai 200062, China
E-mail: ke.qu@siat.ac.cn, zzyang@phy.ecnu.edu.cn

Abstract

The performance of a cathode depends on its microscopic morphology and crystal structure, which are usually affected by the calcination temperature. Herein, we systematically studied the effect of calcination temperature on a novel spherical cobalt-free 0.6Li₂MnO₃·0.4Li[Fe_1/3Ni_1/3Mn_1/3]O₂ (LFNMO) cathode on the three scales of particles, crystal grains and unit cells. The results show that the LFNMO prepared at 850 °C exhibits the highest tap density (2.11 g cm⁻³), the largest I₍₀₀₃₎/I₍₁₀₄₎ (1.3175) and c/a (4.9881) ratios, and the most well-developed layered structure with the least lithium/transition metal (Li/TM) cation mixing. The LFNMO prepared at a lower calcination temperature (800 °C) exhibits low crystallinity, an unbalanced phase ratio, and the poorest layered structure with serious Li/TM cation mixing. The higher temperature (900 °C) causes the overgrowth of primary particles, leading to the growth of ion transport paths and a poorer layered structure with more Li/TM cation mixing, which shows low discharge specific capacity and poor rate capability. The LFNMO cathode prepared at 850 °C shows the best electrochemical performance and exhibits a discharge specific capacity of 213 mA h g⁻¹ at C/10, and the capacity retention rate is 88.3% after 200 cycles. The findings highlight the importance of calcination temperature for the preparation and development of cobalt-free lithium-rich manganese-based cathode materials.

Sustainable Energy & Fuels

Insight into the microscopic morphology and electrochemical performance correlation mechanism upon calcination at different temperatures of a novel spherical cobalt-free 0.6Li₂MnO₃·0.4Li[Fe_1/3Ni_1/3Mn_1/3]O₂ cathode†

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Insight into the microscopic morphology and electrochemical performance correlation mechanism upon calcination at different temperatures of a novel spherical cobalt-free 0.6Li₂MnO₃·0.4Li[Fe_1/3Ni_1/3Mn_1/3]O₂ cathode

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