Please use this identifier to cite or link to this item: https://scholarbank.nus.edu.sg/handle/10635/248298
Title: On the Active Components in Crystalline Li-Nb-O and Li-Ta-O Coatings from First Principles
Authors: Chen, Hengning
Deng, Zeyu 
Li, Yuheng 
Canepa, Pieremanuele 
Keywords: Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Materials Science, Multidisciplinary
Chemistry
Materials Science
X-RAY-DIFFRACTION
LITHIUM-NIOBATE
ELECTRODE MATERIALS
SINGLE-CRYSTALS
CONDUCTIVITY
LINBO3
DEFECTS
LITAO3
PERFORMANCE
CONDUCTORS
Issue Date: 7-Jul-2023
Publisher: AMER CHEMICAL SOC
Citation: Chen, Hengning, Deng, Zeyu, Li, Yuheng, Canepa, Pieremanuele (2023-07-07). On the Active Components in Crystalline Li-Nb-O and Li-Ta-O Coatings from First Principles. CHEMISTRY OF MATERIALS 35 (14) : 5657-5670. ScholarBank@NUS Repository.
Abstract: Layered-oxide LiNixMnyCo1-x-yO2 (NMC) positive electrodes with high nickel content deliver high voltages and energy densities. However, a high nickel content, e.g., x = 0.8 (NMC811), can lead to high surface reactivity, which can trigger thermal runaway and gas generation. While claimed safer, all-solid-state batteries still suffer from high interfacial resistance. Here, we investigate niobate and tantalate coating materials, which can mitigate the interfacial reactivities in Li-ion and all-solid-state batteries. First-principles calculations reveal the multiphasic nature of Li-Nb-O and Li-Ta-O coatings, containing mixtures of LiNbO3 and Li3NbO4 or of LiTaO3 and Li3TaO4. The concurrence of several phases in Li-Nb-O or Li-Ta-O modulates the type of stable native defects in these coatings. Li-Nb-O and Li-Ta-O coating materials can favorably form lithium vacancies VacLi′ and antisite defects NbLi•••• (TaLi••••) combined into charge-neutral defect complexes. Even in defective crystalline LiNbO3 (or LiTaO3), we reveal poor Li-ion conduction properties. In contrast, Li3NbO4 and Li3TaO4 that are introduced by high-temperature calcinations can provide adequate Li-ion transport in these coatings. Our in-depth investigation of the structure-property relationships in the important Li-Nb-O and Li-Ta-O coating materials helps to develop more suitable calcination protocols to maximize the functional properties of these niobates and tantalates.
Source Title: CHEMISTRY OF MATERIALS
URI: https://scholarbank.nus.edu.sg/handle/10635/248298
ISSN: 08974756
15205002
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