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Unveiling the parasitic-reaction-driven surface reconstruction in Ni-rich cathode and the electrochemical role of Li_(2)CO_(3)

引用

Journal of Energy Chemistry 2023年第10期85卷 126-136,I0006页

作者： Jiyu Cai Zhenzhen Yang Xinwei Zhou Bingning Wang Ana Suzana Jianming Bai Chen Liao Yuzi Liu Yanbin Chen Shunlin Song Xuequan Zhang Li Wang Xiangming He Xiangbo Meng Niloofar Karami Baasit Ali Shaik Sulaiman natasha a.chernova Shailesh Upreti Brad Prevel Feng Wang Zonghai Chen Chemical Sciences and Engineering Division Argonne National Laboratory9700 South Cass AvenueLemontIL 60439USA Center for Nanoscale Materials Argonne National Laboratory9700 South Cass AvenueLemontIL 60439USA Condensed Matter Physics and Materials Science Department Brookhaven National LaboratoryUptonNY 11973USA Energy and Photon Sciences Directorate Brookhaven National LaboratoryUptonNY 11973USA Beijing Easprint Material Technology Co.Ltd. Beijing 100160China Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China Department of Mechanical Engineering University of ArkansasFayettevilleAR 72701USA Charge CCCV(C4V) 45 Murray Hill RoadCenter of ExcellenceBinghamton UniversityVestalNY 13850USA Primet Precision Materials 950 Danby RoadIthacaNY 14850USA Applied Materials Division Argonne National Labo

Nickel-rich transition-metal oxides are widely regarded as promising cathode materials for high-energydensity lithium-ion batteries for emerging electric vehicles. However, achieving high energy density in Ni-rich cathodes is accompanied by substantial safety and cycle-life obstacles. The major issues of Ni-rich cathodes at high working potentials are originated from the unstable cathode-electrolyte interface, while the underlying mechanism of parasitic reactions towards surface reconstructions of cathode materials is not well understood. In this work, we controlled the Li_(2)CO_(3) impurity content on LiNi_(0.83)Mn_(0.1)Co_(0.07)O_(2) cathodes using air, tank-air, and O_(2) synthesis environments. Home-built high-precision leakage current and on-line electrochemical mass spectroscopy experiments verify that Li_(2)CO_(3) impurity is a significant promoter of parasitic reactions on Ni-rich cathodes. The rate of parasitic reactions is strongly correlated to Li_(2)CO_(3) content and severe performance deterioration of Ni83 *** post-mortem characterizations via high-resolution transition electron microscope and X-ray photoelectron spectroscopy depth profiles reveal that parasitic reactions promote more Ni reduction and O deficiency and even rock-salt phase transformation at the surface of cathode materials. Our observation suggests that surface reconstructions have a strong affiliation to parasitic reactions that create chemically acidic environment to etch away the lattice oxygen and offer the electrical charge to reduce the valence state of transition metal. Thus, this study advances our understanding on surface reconstructions of Nirich cathodes and prepares us for searching for rational strategies.

关键词： Ni-rich cathodes Surface reconstructions Phase transformation Parasitic reactions Li_(2)CO_(3)

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