Electron and Ion Transfer across Interfaces of the NASICON-Type LATP Solid Electrolyte with Electrodes in All-Solid-State Batteries: A Density Functional Theory Study via an Explicit Interface Model

Hong Kang Tian, Randy Jalem, Bo Gao, Yuta Yamamoto, Shunsuke Muto, Miyuki Sakakura, Yasutoshi Iriyama, Yoshitaka Tateyama

研究成果: Article同行評審

12 引文 斯高帕斯(Scopus)

摘要

NASICON-type oxide Li1+xAlxTi2-x(PO4)3 (LATP) is expected to be a promising solid electrolyte (SE) for all-solid-state batteries (ASSBs) owing to its high ion conductivity and chemical stability. However, its interface properties with electrodes on the atomic scale remain unclear, but it is crucial for rational control of the ASSBs performance. Herein, we focused on the LATP SE with x = 0.17 and investigated the electron and ion transfer behaviors at the interfaces with the Li metal negative electrode and the LiCoO2 (LCO) positive electrode via explicit interface models and density functional theory calculations. Ti reduction was found at the LATP/Li interface. For the LATP/LCO interface, the results indicated the Li-ion transfer from LCO to LATP upon contact until a certain electric double layer is formed under equilibrium, in which LCO is partially reduced. Co-Ti exchange was also found to be favorable where the Li ion moves with Co3+ to LATP. We also explored the possible interfacial processes during annealing by simulating the oxygen removal effect and found that oxygen vacancy can be more easily formed in the LCO at the interface. It implies that partial Li ions move back to LCO for the local charge neutrality. We also demonstrated higher Li chemical potential around the LATP/LCO interfaces, leading to the dynamical Li-ion depletion upon charging. The calculation results and the deduced mechanisms well explain the experimental results so far and provide insights into the interfacial electron and ion transfer upon contact, during annealing, and charging.

原文English
頁(從 - 到)54752-54762
頁數11
期刊ACS Applied Materials and Interfaces
12
發行號49
DOIs
出版狀態Published - 2020 12月 9

All Science Journal Classification (ASJC) codes

  • 材料科學(全部)

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