Abstract

Conformal coating of nm-thick Al2O3 layers on electrode material is an effective strategy for improving the longevity of rechargeable batteries. However, solid understanding of how and why surface coatings work the way they do has yet to be established. In this article, we report on low-temperature atomic layer deposition (ALD) of Al2O3 on practical, ready-to-use composite cathodes of NCM622 (60% Ni), a technologically important material for lithium-ion battery applications. Capacity retention and performance of Al2O3-coated cathodes (≤10 ALD growth cycles) are significantly improved over uncoated NCM622 reference cathodes, even under moderate cycling conditions. Notably, the Al2O3 surface shell is preserved after cycling in full-cell configuration for 1400 cycles as revealed by advanced electron microscopy and elemental mapping. While there are no significant differences in terms of bulk lattice structure and transition-metal leaching among the coated and uncoated NCM622 materials, the surface of the latter is found to be corroded to a much greater extent. In particular, detachment of active material from the secondary particles and side reactions with the electrolyte appear to lower the electrochemical activity, thereby leading to accelerated capacity degradation.

Highlights

  • (Al2O3) is by far the most prominent and widely used, in academia and industry

  • Because the contact points between the CAM secondary particles, the conductive carbon black and the current collector remain free of atomic layer deposition (ALD) material, superior electron and lithium-ion transport properties can be expected for coated electrodes over powder[19,22]

  • NCM622 composite cathodes were coated with Al2O3 using 4, 10 and 40 ALD growth cycles

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Summary

Introduction

(Al2O3) is by far the most prominent and widely used, in academia and industry. ALD offers the possibility to perform the coating directly on ready-to-use electrodes as reported for Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344, Eggenstein-Leopoldshafen, Germany. Several studies reported on reduced transition-metal dissolution after cycling and/or in storage[18,20,22,36]. In agreement with the hypothesis of reduced transition-metal dissolution, lower HF concentrations in the electrolyte were observed for cells using Al2O3-coated cathodes[6,18]. This indicates that aluminum oxide-based surface shells undergo reaction with detrimental HF. There is clearly a lack of long-term performance studies of graphite-based full-cells using ALD-modified CAM under reasonable cycling conditions

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