Atomic layer deposition of lithium zirconium oxides for the improved performance of lithium-ion batteries

Yongqiang Liu; Xin Wang; Sujan Kumar Ghosh; Min Zou; Hua Zhou; Xianghui Xiao; Xiangbo Meng

doi:10.1039/d1dt03600a

Atomic layer deposition of lithium zirconium oxides for the improved performance of lithium-ion batteries

Dalton Trans. 2022 Feb 14;51(7):2737-2749. doi: 10.1039/d1dt03600a.

Authors

Yongqiang Liu^{1

2}, Xin Wang¹, Sujan Kumar Ghosh^{1

3}, Min Zou^{1

3}, Hua Zhou⁴, Xianghui Xiao⁵, Xiangbo Meng^{1

3}

Affiliations

¹ Department of Mechanical Engineering, The University of Arkansas, Fayetteville, AR 72701, USA. xbmeng@uark.edu.
² College of Science, Northeast Forestry University, Harbin 150040, Heilongjiang, China.
³ The Center for Advanced Surface Engineering, The University of Arkansas, Fayetteville, AR 72701, USA.
⁴ Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
⁵ National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973, USA. xiao@bnl.gov.

PMID: 35112679
DOI: 10.1039/d1dt03600a

Abstract

Recently there has been increasing interest to develop lithium-containing films as solid-state electrolytes or surface coatings for lithium-ion batteries (LIBs) and related systems. In this study, we for the first time investigated the thin film growth of lithium zirconium oxides (Li_xZr_yO or LZOs) through combining two individual atomic layer deposition (ALD) processes of ZrO₂ and LiOH, i.e., sub-ALD of ZrO₂ and LiOH. We revealed that the hygroscopic nature of the LiOH component has a big impact on the growth of LZOs. We found that an increased temperature to 225 °C was more effective than an elongated purge to mitigate the adverse effects of physisorbed H₂O. We further discovered that, during the resultant LZO super-ALD processes, the growth of sub-ALD LiOH has been promoted while the growth of sub-ALD ZrO₂ has been inhibited. In this study, a suite of instruments has been applied to characterize the LZO super-ALD processes and the resultant LZO films, including in situ quartz crystal microbalance (QCM), scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM), atomic force microscopy (AFM), synchrotron-based X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Furthermore, we applied the resulting LZO films over LiNi_0.6Mn_0.2Co_0.2O₂ (NMC622) cathodes in LIBs and demonstrated that the LZO coating films could evidently improve the lithium-ion insertion and extraction rates of the NMC622 electrodes up to 3.4 and 2.6 times, respectively. The LZO-coated NMC622 cathodes exhibited much better performance than the uncoated NMC622 ones.