In Situ Induced Surface Reconstruction of Single-Crystal Lithium-Ion Cathode Toward Effective Interface Compatibility
journal contributionposted on 11.03.2021, 17:04 by Qingqing Zhang, Kai Liu, Cheng Li, Lu Li, Xingjiang Liu, Wei Li, Jinli Zhang
LiNixCoyMn1–x–yO2 (x ≥ 0.5) layered oxide materials are generally considered as one of the most prospective candidates for lithium-ion battery (LIBs) cathodes due to their high specific capacity and working voltage. However, surface impurity species substantially degrade the electrochemical performance of LIBs. Herein, surface reconstruction from layered structure to disordered layer and rock-salt coherent region together with a uniform Li2CO3-dominant coating layer is first in situ constructed on the single-crystal LiNi0.5Co0.2Mn0.3O2 (NCM) material by a simple water treatment procedure. The unique surface structure is elucidated by Ar-sputtering-assisted X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (spherical aberration-corrected-scanning transmission electron microscopy (STEM), high-resolution transmission electron microscopy (HRTEM), and TEM). Meanwhile, neutron powder diffraction (NPD) indicates that the antisite defect concentration is mitigated in the treated materials. The modified samples display superior cycle stability with a capacity retention of up to 87.5% at 1C after 300 cycles, a high rate capacity of 151 mAh g–1 at 5C, an elevated temperature (45 °C) cycling property with 80% capacity retention (4.5 V), and improved full-cell performance with 91% after 250 cycles at 1C. Importantly, postmortem examination on the cycled cathodes by time-of-flight secondary-ion mass spectroscopy (TOF-SIMS), XPS, TEM, and X-ray diffractometer (XRD) pattern further demonstrate that these results are mainly attributed to the thin cathode electrolyte interface (CEI) film and low solubility of transition-metal ions. Therefore, this expedition provides an opportunity to construct an effective armor for the interface compatibility and stability of LIBs.
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LIBAr-sputtering-assisted X-ray photoe...stability1 CretentionTOF-SIMSmaterialneutron powder diffractionXPSHRTEMNPDCEIXRDuniform Li 2 CO 3time-of-flight secondary-ion mass s...antisite defect concentrationsingle-crystal LiNi 0.5 Co 0.2 Mn 0...TEMwater treatment proceduretransmission electron microscopySitu Induced Surface ReconstructionSingle-Crystal Lithium-Ion Cathodeaberration-corrected-scanning trans...cathode electrolyte interfaceperformancesurface impurity speciescapacityNCM