Xiao, Yuanbin, Zhang, Weicheng, Dong, Weikang, Yang, Kang, Chao, Yu, Xi, Chenpeng, Li, Mengchao, Zhang, Qiaoli, Liu, Zheyuan, Du, Peng, Liu, Huan, Zhang, Weidong, Shao, Ruiwen, Wang, Qian, Yu, Yan, and Yang, Chengkai
• A dissociated solvation cluster dominated by NO 3 − is proposed to regulate the effects of cathode interface phase transition and cyclic fragmentation. Existing methods, including our previous work, typically study the effects on the anode interface structure, which are difficult to solve the interface problem generated by the cathode. Thus, we have developed a unique approach to enhance the solubility of LiNO 3 in carbonate electrolyte systems by employing a novel local high-concentrated addition strategy with triethyl phosphate (TEP) as a co-solvent. • Distinct solvation clusters are constructed in NO 3 − dominated electrolyte. Here, Our research focuses on dissociative solvation clusters dominated by NO 3 −, by studying the specific complexation behavior of NO 3 − and Li+. there are two distinct solventization clusters. One is the PF 6 − dominated solvation cluster (PSC) while the FEC is distributed in the outer layer with a loose solvation, and the other is the tight NO 3 − dominated solvation cluster (NSC). The NSC has weak ionization and fast diffusion properties. The PSC also has a reduced binding energy and increased coordination distance Adjacent to NSC. It is attributed to the interactions induced by the TEP and the DMC/FEC in PSC. Thus, the coordination environment of PSC is further loosened, leading to the enhanced diffusion ability of Li+ and PF 6 −, which affects the cathode-electrolyte interface process between the cathode and electrolyte. • The tight NO 3 − dominated solvation cluster improves the electrochemical kinetics process. The uniformly distributed induced Li-N composite interfacial CEI layer generated by the tight NO 3 − dominated solvation cluster accelerates the interfacial Li+ conduction, improves the stability of the interfacial interface, and effectively inhibits the phase transition and stress fracture in the charge–discharge process. • Achieving excellent compatibility with high-voltage NCM cathodes and an excellent electrochemical performance. Stable coulombic efficiency and improved cycling stability were achieved. Full battery cycle performance using NCM811 cathode 0.5C initial discharge specific capacity up to 189 mAh/g, after 300 cycles still has 152 mAh/g discharge specific capacity, capacity retention rate of 80%. The specific discharge capacity of 165 mAh/g is still available under high magnification test conditions (5C). To meet the demand for higher energy density in lithium-ion batteries, extensive research has focused on advanced cathodes and metallic lithium anodes. However, Ni-rich cathodes suffer from the inactive phase-transition and side reactions at the cathode-electrolyte interfaces (CEI). In this study, we propose a novel approach to enhance the solubility of LiNO 3 in carbonate electrolyte systems using a local high-concentrated addition strategy with triethyl phosphate as a co-solvent. Rather than the traditional solvent-dominated solvation clusters, the NO 3 − dominated electrolyte is examined to elucidate unique complexation phenomena. Two distinct clusters in NO 3 − dominated electrolyte arising from as a consequence of intramolecular interactions intrinsic to the constituents. This promotes the formation of a homogeneous oxynitride interphase and facilitates more expeditious lithium ion diffusion kinetics. Hence, the less stress fragmentation and irreversible phase transformation occur on the cathode surface with the homogeneous oxynitridation interface. This innovative design enables efficient cycling of the Li || NCM811 cell, offering a promising strategy to improve lithium-ion batteries performance. [ABSTRACT FROM AUTHOR]