Enhanced Cycling Performance of Spinel LiNi_0.5Mn_1.5O₄ Cathodes through Mg-Mn Hetero-Valent Doping via Microwave...

As a high energy density cathode material, further development of high working voltage spinel LiNi_0.5Mn_1.5O₄ has hindered by its rapid capacity degradation. To address this, a hetero-valent substitution of magnesium for manganese was used to synthesize spinel LiNi0.5Mg_xMn_1.5-xO₄ (x = 0, 0.03, 0.05) via a microwave sol-gel method. XRD and refined results indicate that such strategy leads to the modification of the 16c interstitial sites. The electrical performance demonstrates that a modest substitution (x = 0.03) significantly improves both rate performance (113.1 mAh/g, charge and discharge at 5 C) and cycling stability (85% capacity retention after 500 cycles at 1 C). A higher substitution level (x = 0.05) markedly improves high-rate cycling performance, achieving 96% capacity retention after 500 cycles at 5 C. It offers tailored solutions for various application needs, including capacity-focused and high-current-rate applications. Furthermore, the stable LiNi_0.5Mg_0.05Mn_1.45O₄ sample could also serve as an effective coating layer for other electrode materials to enhance their cycling stability.