Understanding Performance Differences from Various Synthesis Methods: A Case Study of Spinel LiCr_0.2Ni_0.4Mn_1.4O₄ Cathode Material

High voltage (5-V class) spinel LiCr_0.2Ni_0.4Mn_1.4O₄ is one of the most promising cathode materials to meet the energy requirements of lithium-ion batteries for electric vehicles and hybrid electric vehicles. For the mass production of this material (1 kg or higher), different synthesis routes will lead to different electrochemical performances, even with similar morphology and similar crystal structure obtained from laboratory X-ray diffraction, and the reason for this issue is still not clear. Herein, we have investigated the reasons for the different electrochemical performances resulting from three common synthesis routes (spray pyrolysis, coprecipitation, and sol-gel). Taking advantage of the high-resolution X-ray beam in synchrotron X-ray diffraction, we find that varying phase composition and the generated impurities, rather than the particle distribution, are likely to be the main reasons for the detected electrochemical variations. A higher amount of impurities will result in greater charge transfer resistance, inferior cycling stability, and more oxygen/lithium vacancies. Therefore, it is very important to obtain a deeper understanding with the help of higher-resolution X-rays and to provide better guidance for mass production of this cathode material for practical applications.