Identifying the Distribution of Al 3+ in LiNi 0.8 Co 0.15 Al 0.05 O 2
Abstract
The doping of Al into layered Li transition metal (TM) oxide cathode materials, LiTMO2, is known to improve the structural and thermal stability, although the origin of the enhanced properties is not well understood. We have investigated the effect of aluminum doping on layer stabilization using a combination of techniques to measure the aluminum distribution in layered LiNi0.8Co0.15Al0.05O2 (NCA) over multiple length scales with 27Al and 7Li MAS NMR, local electron atom probe (LEAP) tomography, X-ray and neutron diffraction, DFT, and SQUID magnetic susceptibility measurements. LEAP tomographic maps show a homogenous distribution of Ni, Co, Al and O2 throughout the structure at the particle level in agreement with the hightemperature phase diagram. 7Li and 27Al NMR indicates that the Ni3+ ions undergo a dynamic Jahn-Teller (JT) distortion. 27Al NMR spectra indicate that the Al reduces the strain associated with the JT distortion, by preferential electronic ordering of the JT long bonds directed toward the Al3+ ion. Our ability to understand the complex atomic and orbital ordering around Al3+ demonstrated in the current method will be useful for studying the local environment of Al3+ in a range of transition metal oxide battery materials.
- Authors:
-
- Univ. of Cambridge (United Kingdom). Dept. of Chemistry
- Univ. of California, Santa Barbara, CA (United States). Materials Dept.
- Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
- State Univ. of New York (SUNY), Binghamton, NY (United States). Inst. for Materials Research
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1378325
- Grant/Contract Number:
- AC02-06CH11357; SC0012583; AC05-76RL01830; SC0001294
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 28; Journal Issue: 22; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 27 Al NMR; NCA; atom probe tomography; dynamic Jahn-Teller; paramagnetic NMR
Citation Formats
Trease, Nicole M., Seymour, Ieuan D., Radin, Maxwell D., Liu, Haodong, Liu, Hao, Hy, Sunny, Chernova, Natalya, Parikh, Pritesh, Devaraj, Arun, Wiaderek, Kamila M., Chupas, Peter J., Chapman, Karena W., Whittingham, M. Stanley, Meng, Ying Shirley, Van der Van, Anton, and Grey, Clare P. Identifying the Distribution of Al 3+ in LiNi 0.8 Co 0.15 Al 0.05 O 2. United States: N. p., 2016.
Web. doi:10.1021/acs.chemmater.6b02797.
Trease, Nicole M., Seymour, Ieuan D., Radin, Maxwell D., Liu, Haodong, Liu, Hao, Hy, Sunny, Chernova, Natalya, Parikh, Pritesh, Devaraj, Arun, Wiaderek, Kamila M., Chupas, Peter J., Chapman, Karena W., Whittingham, M. Stanley, Meng, Ying Shirley, Van der Van, Anton, & Grey, Clare P. Identifying the Distribution of Al 3+ in LiNi 0.8 Co 0.15 Al 0.05 O 2. United States. https://doi.org/10.1021/acs.chemmater.6b02797
Trease, Nicole M., Seymour, Ieuan D., Radin, Maxwell D., Liu, Haodong, Liu, Hao, Hy, Sunny, Chernova, Natalya, Parikh, Pritesh, Devaraj, Arun, Wiaderek, Kamila M., Chupas, Peter J., Chapman, Karena W., Whittingham, M. Stanley, Meng, Ying Shirley, Van der Van, Anton, and Grey, Clare P. Fri .
"Identifying the Distribution of Al 3+ in LiNi 0.8 Co 0.15 Al 0.05 O 2". United States. https://doi.org/10.1021/acs.chemmater.6b02797. https://www.osti.gov/servlets/purl/1378325.
@article{osti_1378325,
title = {Identifying the Distribution of Al 3+ in LiNi 0.8 Co 0.15 Al 0.05 O 2},
author = {Trease, Nicole M. and Seymour, Ieuan D. and Radin, Maxwell D. and Liu, Haodong and Liu, Hao and Hy, Sunny and Chernova, Natalya and Parikh, Pritesh and Devaraj, Arun and Wiaderek, Kamila M. and Chupas, Peter J. and Chapman, Karena W. and Whittingham, M. Stanley and Meng, Ying Shirley and Van der Van, Anton and Grey, Clare P.},
abstractNote = {The doping of Al into layered Li transition metal (TM) oxide cathode materials, LiTMO2, is known to improve the structural and thermal stability, although the origin of the enhanced properties is not well understood. We have investigated the effect of aluminum doping on layer stabilization using a combination of techniques to measure the aluminum distribution in layered LiNi0.8Co0.15Al0.05O2 (NCA) over multiple length scales with 27Al and 7Li MAS NMR, local electron atom probe (LEAP) tomography, X-ray and neutron diffraction, DFT, and SQUID magnetic susceptibility measurements. LEAP tomographic maps show a homogenous distribution of Ni, Co, Al and O2 throughout the structure at the particle level in agreement with the hightemperature phase diagram. 7Li and 27Al NMR indicates that the Ni3+ ions undergo a dynamic Jahn-Teller (JT) distortion. 27Al NMR spectra indicate that the Al reduces the strain associated with the JT distortion, by preferential electronic ordering of the JT long bonds directed toward the Al3+ ion. Our ability to understand the complex atomic and orbital ordering around Al3+ demonstrated in the current method will be useful for studying the local environment of Al3+ in a range of transition metal oxide battery materials.},
doi = {10.1021/acs.chemmater.6b02797},
journal = {Chemistry of Materials},
number = 22,
volume = 28,
place = {United States},
year = {2016},
month = {10}
}
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