Advanced TiO2/Al2O3 Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

Wei-Ming Chen; Hsin-Yu Hsieh; Dong-Ze Wu; Horng-Yi Tang; Kuei-Shu Chang-Liao; Po-Wei Chi; Phillip M Wu; Maw-Kuen Wu

doi:10.1021/acsami.3c16948

Advanced TiO₂/Al₂O₃ Bilayer ALD Coatings for Improved Lithium-Rich Layered Oxide Electrodes

ACS Appl Mater Interfaces. 2024 Mar 13;16(10):13029-13040. doi: 10.1021/acsami.3c16948. Epub 2024 Feb 29.

Authors

Wei-Ming Chen^{1

2

3}, Hsin-Yu Hsieh¹, Dong-Ze Wu^{1

4}, Horng-Yi Tang⁵, Kuei-Shu Chang-Liao³, Po-Wei Chi¹, Phillip M Wu^{1

6}, Maw-Kuen Wu¹

Affiliations

¹ Institute of Physics, Academia Sinica, 128, Section 2, Academia Road, Taipei 11529, Taiwan.
² Nano Science and Technology Program, Taiwan International Graduate Program, Academia Sinica and National Tsing Hua University, 128, Section 2, Academia Road, Taipei 11529, Taiwan.
³ Department of Engineering and System Science, National Tsing Hua University, 101, Section 2, Kuang-Fu Road, Hsinchu 300044, Taiwan.
⁴ Graduate Institute of Energy and Sustainability Technology, National Taiwan University of Science and Technology, 43 Keelung Road, Sec 4, Taipei 10607, Taiwan.
⁵ Department of Applied Chemistry, National Chi Nan University, 1 University Road, Puli, Nantou 545301, Taiwan.
⁶ College of Science, National Chung Hsing University, 145 Xingda Rd., South Dist., Taichung City 402, Taiwan.

Abstract

Surface modification is a highly effective strategy for addressing issues in lithium-rich layered oxide (LLO) cathodes, including phase transformation, particle cracking, oxygen gas release, and transition-metal ion dissolution. Existing single-/double-layer coating strategies face drawbacks such as poor component contact and complexity. Herein, we present the results of a low-temperature atomic layer deposition (ALD) process for creating a TiO₂/Al₂O₃ bilayer on composite cathodes made of AS200 (Li_1.08Ni_0.34Co_0.08Mn_0.5O₂). Electrochemical analysis demonstrates that TiO₂/Al₂O₃-coated LLO electrodes exhibit improved discharge capacities and enhanced capacity retention compared with uncoated samples. The TAA-5/AS200 bilayer-coated electrode, in particular, demonstrates exceptional capacity retention (∼90.4%) and a specific discharge capacity of 146 mAh g^-1 after 100 cycles at 1C within the voltage range of 2.2 to 4.6 V. The coated electrodes also show reduced voltage decay, lower surface film resistance, and improved interfacial charge transfer resistances, contributing to enhanced stability. The ALD-deposited TiO₂/Al₂O₃ bilayer coatings exhibit promising potential for advancing the electrochemical performance of lithium-rich layered oxide cathodes in lithium-ion batteries.

Keywords: atomic layer deposition; lithium-ion battery; lithium-rich cathode; surface modification; thin film.