TY - JOUR
T1 - Atomic-Scale Mechanisms of Enhanced Electrochemical Properties of Mo-Doped Co-Free Layered Oxide Cathodes for Lithium-Ion Batteries
AU - Li, Linze
AU - Yu, Jianguo
AU - Darbar, Devendrasinh
AU - Self, Ethan C.
AU - Wang, Donghai
AU - Nanda, Jagjit
AU - Bhattacharya, Indranil
AU - Wang, Chongmin
N1 - Funding Information:
This work is supported by the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technology Office, under Award Number DE-EE0008447. The work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE’s Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the Department of Energy under Contract DE-AC05-76RLO1830. Scanning electron microscopy was conducted at the Center for Nanophase Materials Science, which is a DOE Office of Science User Facility.
Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/8/20
Y1 - 2019/8/20
N2 - Cobalt-free layered oxides have emerged as promising candidates for next-generation cathodes for lithium-ion batteries. However, implementation of these materials has been hindered by their low rate capability, structural instability, and rapid capacity decay during cycling. Recent studies have shown that introducing cation dopants into layered oxides can strongly improve their electrochemical properties, but the underlying atomic-scale mechanisms remain elusive. In this work, we use a combination of atomic-resolution scanning transmission electron microscopy and first-principle calculations to reveal the microscopic origin of enhanced electrochemical properties in LiNi0.5Mn0.5O2 doped with ∼1 atom % Mo. Our results indicate that the Mo dopant hinders Li+/Ni2+ cation mixing and suppresses detrimental phase transformations near the particle surface and at intragranular grain boundaries, which enhances the cathode's reversible capacity and cycling stability. Overall, this work provides important insights on how cation doping affects the structure and electrochemical properties of layered oxide cathodes.
AB - Cobalt-free layered oxides have emerged as promising candidates for next-generation cathodes for lithium-ion batteries. However, implementation of these materials has been hindered by their low rate capability, structural instability, and rapid capacity decay during cycling. Recent studies have shown that introducing cation dopants into layered oxides can strongly improve their electrochemical properties, but the underlying atomic-scale mechanisms remain elusive. In this work, we use a combination of atomic-resolution scanning transmission electron microscopy and first-principle calculations to reveal the microscopic origin of enhanced electrochemical properties in LiNi0.5Mn0.5O2 doped with ∼1 atom % Mo. Our results indicate that the Mo dopant hinders Li+/Ni2+ cation mixing and suppresses detrimental phase transformations near the particle surface and at intragranular grain boundaries, which enhances the cathode's reversible capacity and cycling stability. Overall, this work provides important insights on how cation doping affects the structure and electrochemical properties of layered oxide cathodes.
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U2 - 10.1021/acsenergylett.9b01830
DO - 10.1021/acsenergylett.9b01830
M3 - Article
AN - SCOPUS:85073145878
VL - 4
SP - 2540
EP - 2546
JO - ACS Energy Letters
JF - ACS Energy Letters
SN - 2380-8195
IS - 10
ER -