Affiliation:
1. School of Metallurgy and Environment Central South University Changsha 410083 P. R. China
2. Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South University Changsha 410083 P. R. China
3. State Key Lab for Phys Chemistry of Solid Surfaces & Department of Chemistry Xiamen University Xiamen 361005 P. R. China
4. Changsha Research Institute of Mining and Metallurgy Changsha 410083 P. R. China
5. Institute of Nanotechnology Karlsruhe Institute of Technology (KIT) 76344 Eggenstein‐Leopoldshafen Germany
Abstract
AbstractIntergranular cracking of Ni‐rich layered LiNi1‐x‐yCoxMnyO2 (1‐x‐y ≥ 0.8) cathode particles deteriorate the chemo–electro–mechanical stability of high‐energy lithium‐ion batteries (LIBs), thus presenting a challenge to typical modification methods to establish robust structures with highly efficient lithium‐ion storage. Herein, the ZrTiO4 (ZTO) as an epitaxial layer to enhance mechanical stability of ultrahigh‐Ni LiNi0.9Co0.05Mn0.05O2 (NCM90) is reported for the first time. Intensive exploration from structure characterizations (X‐ray absorption spectroscopy and in situ X‐ray diffraction techniques), multi‐physics field analysis, and first‐principles calculations disclose that the conformal ZTO layers and Zr doping effectively suppresses the internal strain and the release of lattice oxygen, which prodigiously restrains the local stress accumulation during whole (de)lithiation processes, thereby maintaining good mechanical stability of the materials. Meanwhile, the protective ZTO layer also prevents electrolyte erosion, thus keeping an intact surface structure of NCM90. Notably, ZTO‐modified NCM90 achieves significantly improved cyclability under high‐voltage (4.5 V) operation, expressing a 17% increase in capacity retention (71% vs 88%) after 100 cycles. Overall, this work reveals the role of internal strain in the original degradation behavior and effectiveness of surface engineering strategy to solve the challenge, emphasizing that the conformal surface protection mitigates the internal stress of Ni‐rich NCM by anchoring the lattice oxygen.
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials
Cited by
45 articles.
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