Abstract
We present a structural and magnetic study of two batches of polycrystalline LiNi0.8Mn0.1Co0.1O2 (commonly known as Li NMC 811), a Ni-rich Li ion battery cathode material, using elemental analysis, X-ray and neutron diffraction, magnetometry, and polarized neutron scattering measurements. We find that the samples, labeled S1 and S2, have the composition Li1-xNi0.9+x-yMnyCo0.1O2, with x = 0.025(2), y = 0.120(2) for S1 and x = 0.002(2), y = 0.094(2) for S2, corresponding to different concentrations of magnetic ions and excess Ni2+ in the Li+ layers. Both samples show a peak in the zero-field-cooled (ZFC) dc susceptibility at 8.0(2) K, but the temperature at which the ZFC and FC (field-cooled) curves deviate is substantially different: 64(2) K for S1 and 122(2) K for S2. The ac susceptibility measurements show that the transition for S1 shifts with frequency whereas no such shift is observed for S2 within the resolution of our measurements. Our results demonstrate the sample dependence of magnetic properties in Li NMC 811, consistent with previous reports on the parent material LiNiO2. We further establish that a combination of experimental techniques is necessary to accurately determine the chemical composition of next-generation battery materials with multiple cations.
Original language | English |
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Pages (from-to) | 263-271 |
Number of pages | 9 |
Journal | Inorganic Chemistry |
Volume | 60 |
Issue number | 1 |
DOIs | |
State | Published - Jan 4 2021 |
Funding
We thank the Science and Technology Facilities Council (STFC) for provision of ISIS Xpress Access beam time on GEM and the Institut Laue-Langevin for allocation of EASY beam time on D7. P.M., C.X., Z.R., C.P.G., and S.E.D. acknowledge funding support from the Faraday Institution EPSRC Grant EP/S003053/1. Magnetic measurements were performed by using the Advanced Materials Characterisation Suite, funded by EPSRC Strategic Equipment Grant EP/M000524/1. We thank Cheng Liu for support with the MPMS and PPMS equipment. We thank Craig A. Bridges (ORNL) and Binod Rai (ORNL) for useful feedback. J.A.M.P.’s work at Cambridge (contribution to neutron data reduction) was supported by Churchill College, University of Cambridge. J.A.M.P.’s work at ORNL was supported by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT- Battelle, LLC, for the US Department of Energy (contribution to data analysis). This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Supporting data can be found at https://doi.org/10.17863/CAM.62029 . Neutron scattering data can also be found at ISIS dois: 10.5286/ISIS.E.RB1890370-1 , 10.5286/ISIS.E.101124089 , and ILL doi: https://doi.ill.fr/10.5291/ILL-DATA.EASY-432 .