Kinetics Tuning of Li-Ion Diffusion in Layered Li(Ni _x Mn _y Co _z )O ₂

Journal Article · Wed Jul 08 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b04040· OSTI ID:1274890

Wei, Yi; Zheng, Jiaxin; Cui, Suihan; Song, Xiaohe; Su, Yantao; Deng, Wenjun; Wu, Zhongzhen; Wang, Xinwei; Wang, Weidong; Rao, Mumin; Lin, Yuan; Wang, Chongmin; Amine, Khalil; Pan, Feng

Using ab initio calculations combined with experiments, we clarified how the kinetics of Li-ion diffusion can be tuned in LiNixMnyCozO2 (NMC, x + y + z = 1) materials. It is found that Li-ions tend to choose oxygen dumbbell hopping (ODH) at the early stage of charging (delithiation), and tetrahedral site hopping (TSH) begins to dominate when more than 1/3 Li-ions are extracted. In both ODH and TSH, the Li-ions surrounded by nickel (especially with low valence state) are more likely to diffuse with low activation energy and form an advantageous path. The Li slab space, which also contributes to the effective diffusion barriers, is found to be closely associated with the delithiation process (Ni oxidation) and the contents of Ni, Co, and Mn.

• Research Organization: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1274890
• Report Number(s): PNNL-SA-113150; KP1704020
• Journal Information: Journal of the American Chemical Society, Vol. 137, Issue 26; ISSN 0002-7863
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English