4.7 Article

Improvement of the Interface between the Lithium Anode and a Garnet-Type Solid Electrolyte of Lithium Batteries Using an Aluminum-Nitride Layer

Journal

NANOMATERIALS
Volume 12, Issue 12, Pages -

Publisher

MDPI
DOI: 10.3390/nano12122023

Keywords

LLZTO; solid-state electrolytes; lithium; electrolyte interface; anode interface; lithium-ion battery

Funding

  1. National Natural Science Foundation of China [51574160, 21776175]
  2. National Key Research and Development Program of China [2017YFB0102004]
  3. Shandong Province National Natural Science Foundation [ZR2014EEM049]
  4. Key Research and Development Program of Shandong Province [2017CSGC0502, 2017GGX40102]
  5. Leading Talents Project: Science and Technology Talents and Platform Plan-training of Science and Technology Talent [2017HA012]
  6. State Key Laboratory of Pressure Hydrometallurgical Technology of Associated Nonferrous Metal Resources [yy20160010]

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In this study, the introduction of an aluminum nitride (AlN) layer improved the interface between lithium and the solid electrolyte, enhancing lithium-ion transport and improving the cycling stability of the battery.
The next generation of all-solid-state batteries can feature battery safety that is unparalleled among conventional liquid batteries. The garnet-type solid-state electrolyte Li7La3Zr2O12 (LLZO), in particular, is widely studied because of its high Li-ion conductivity and stability in air. However, the poor interface-contact between Li and the electrolyte (garnet) severely limits the development of solid electrolytes. In this study, we synthesize cubic phase Li6.4La3Zr1.4Ta0.6O12 (LLZTO) using a secondary sintering method. In addition, a thin aluminum nitride (AlN) layer is introduced between the metal (Li) and the solid electrolyte. Theoretical calculations show that AlN has a high affinity for Li. Furthermore, it is shown that the AlN coating can effectively reduce the interface impedance between Li and the solid electrolyte and improve the lithium-ion transport. The assembled symmetric Li cells can operate stably for more than 3600 h, unlike the symmetric cells without AlN coating, which short-circuited after only a few cycles. The hybrid solid-state battery with a modified layer, which is assembled using LiFePO4 (LFP), still has a capacity of 120 mAh g(-1) after 200 cycles, with a capacity retention rate of 98%. This shows that the introduction of an AlN interlayer is very helpful to obtain a stable Li/solid-electrolyte interface, which improves the cycling stability of the battery.

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