Structural changes and thermal stability of charged LiNixMnyCozO2 cathode materials studied by combined in situ time-resolved XRD and mass spectroscopy
Abstract
Thermal stability of charged LiNixMnyCozO2 (NMC, with x + y + z = 1, x:y:z = 4:3:3 (NMC433), 5:3:2 (NMC532), 6:2:2 (NMC622), and 8:1:1 (NMC811)) cathode materials is systematically studied using combined in situ time- resolved X-ray diffraction and mass spectroscopy (TR-XRD/MS) techniques upon heating up to 600 °C. The TR-XRD/MS results indicate that the content of Ni, Co, and Mn significantly affects both the structural changes and the oxygen release features during heating: the more Ni and less Co and Mn, the lower the onset temperature of the phase transition (i.e., thermal decomposition) and the larger amount of oxygen release. Interestingly, the NMC532 seems to be the optimized composition to maintain a reasonably good thermal stability, comparable to the low-nickel-content materials (e.g., NMC333 and NMC433), while having a high capacity close to the high-nickel-content materials (e.g., NMC811 and NMC622). The origin of the thermal decomposition of NMC cathode materials was elucidated by the changes in the oxidation states of each transition metal (TM) cations (i.e., Ni, Co, and Mn) and their site preferences during thermal decomposition. It is revealed that Mn ions mainly occupy the 3a octahedral sites of a layered structure (R3¯m) but Co ions prefer to migratemore »
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Johnson Control Advanced Power Solution, Milwaukee, WI (United States); North Carolina A&T State Univ., Greensboro, NC (United States)
- Yonsei Univ., Seoul (Republic of Korea)
- Korea Institute of Science and Technology (KIST), Seoul (Republic of Korea)
- Dongguk Univ., Seoul (Republic of Korea)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- OSTI Identifier:
- 1169557
- Report Number(s):
- BNL-107164-2014-JA
Journal ID: ISSN 1944-8244; VT1201000-05450-1005554
- Grant/Contract Number:
- AC02-98CH10886; 2V03693
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 24; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; sodium-ion battery; cathode materials; X-ray absorption spectroscopy; transmission electron microscopy; NSLS; electrode material; energy storage; reaction mechanism
Citation Formats
Bak, Seong -Min, Hu, Enyuan, Zhou, Yongning, Yu, Xiqian, Senanayake, Sanjaya D., Cho, Sung -Jin, Kim, Kwang -Bum, Chung, Kyung Yoon, Yang, Xiao -Qing, and Nam, Kyung -Wan. Structural changes and thermal stability of charged LiNixMnyCozO2 cathode materials studied by combined in situ time-resolved XRD and mass spectroscopy. United States: N. p., 2014.
Web. doi:10.1021/am506712c.
Bak, Seong -Min, Hu, Enyuan, Zhou, Yongning, Yu, Xiqian, Senanayake, Sanjaya D., Cho, Sung -Jin, Kim, Kwang -Bum, Chung, Kyung Yoon, Yang, Xiao -Qing, & Nam, Kyung -Wan. Structural changes and thermal stability of charged LiNixMnyCozO2 cathode materials studied by combined in situ time-resolved XRD and mass spectroscopy. United States. https://doi.org/10.1021/am506712c
Bak, Seong -Min, Hu, Enyuan, Zhou, Yongning, Yu, Xiqian, Senanayake, Sanjaya D., Cho, Sung -Jin, Kim, Kwang -Bum, Chung, Kyung Yoon, Yang, Xiao -Qing, and Nam, Kyung -Wan. Mon .
"Structural changes and thermal stability of charged LiNixMnyCozO2 cathode materials studied by combined in situ time-resolved XRD and mass spectroscopy". United States. https://doi.org/10.1021/am506712c. https://www.osti.gov/servlets/purl/1169557.
@article{osti_1169557,
title = {Structural changes and thermal stability of charged LiNixMnyCozO2 cathode materials studied by combined in situ time-resolved XRD and mass spectroscopy},
author = {Bak, Seong -Min and Hu, Enyuan and Zhou, Yongning and Yu, Xiqian and Senanayake, Sanjaya D. and Cho, Sung -Jin and Kim, Kwang -Bum and Chung, Kyung Yoon and Yang, Xiao -Qing and Nam, Kyung -Wan},
abstractNote = {Thermal stability of charged LiNixMnyCozO2 (NMC, with x + y + z = 1, x:y:z = 4:3:3 (NMC433), 5:3:2 (NMC532), 6:2:2 (NMC622), and 8:1:1 (NMC811)) cathode materials is systematically studied using combined in situ time- resolved X-ray diffraction and mass spectroscopy (TR-XRD/MS) techniques upon heating up to 600 °C. The TR-XRD/MS results indicate that the content of Ni, Co, and Mn significantly affects both the structural changes and the oxygen release features during heating: the more Ni and less Co and Mn, the lower the onset temperature of the phase transition (i.e., thermal decomposition) and the larger amount of oxygen release. Interestingly, the NMC532 seems to be the optimized composition to maintain a reasonably good thermal stability, comparable to the low-nickel-content materials (e.g., NMC333 and NMC433), while having a high capacity close to the high-nickel-content materials (e.g., NMC811 and NMC622). The origin of the thermal decomposition of NMC cathode materials was elucidated by the changes in the oxidation states of each transition metal (TM) cations (i.e., Ni, Co, and Mn) and their site preferences during thermal decomposition. It is revealed that Mn ions mainly occupy the 3a octahedral sites of a layered structure (R3¯m) but Co ions prefer to migrate to the 8a tetrahedral sites of a spinel structure (Fd3¯m) during the thermal decomposition. Such element-dependent cation migration plays a very important role in the thermal stability of NMC cathode materials. The reasonably good thermal stability and high capacity characteristics of the NMC532 composition is originated from the well-balanced ratio of nickel content to manganese and cobalt contents. As a result, this systematic study provides insight into the rational design of NMC-based cathode materials with a desired balance between thermal stability and high energy density.},
doi = {10.1021/am506712c},
journal = {ACS Applied Materials and Interfaces},
number = 24,
volume = 6,
place = {United States},
year = {Mon Nov 24 00:00:00 EST 2014},
month = {Mon Nov 24 00:00:00 EST 2014}
}
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- Sharifi‐Asl, Soroosh; Lu, Jun; Amine, Khalil
- Advanced Energy Materials, Vol. 9, Issue 22
Comparison of Single Crystal and Polycrystalline LiNi 0.5 Mn 0.3 Co 0.2 O 2 Positive Electrode Materials for High Voltage Li-Ion Cells
journal, January 2017
- Li, Jing; Cameron, Andrew R.; Li, Hongyang
- Journal of The Electrochemical Society, Vol. 164, Issue 7
Li[Ni 0.9 Co 0.09 W 0.01 ]O 2 : A New Type of Layered Oxide Cathode with High Cycling Stability
journal, October 2019
- Ryu, Hoon‐Hee; Park, Kang‐Joon; Yoon, Dae Ro
- Advanced Energy Materials, Vol. 9, Issue 44
Evolution of redox couples in Li- and Mn-rich cathode materials and mitigation of voltage fade by reducing oxygen release
journal, July 2018
- Hu, Enyuan; Yu, Xiqian; Lin, Ruoqian
- Nature Energy, Vol. 3, Issue 8
Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries
journal, April 2019
- de Biasi, Lea; Schwarz, Björn; Brezesinski, Torsten
- Advanced Materials, Vol. 31, Issue 26
Amorphous Ni‐Rich Li(Ni 1− x − y Mn x Co y )O 2 –Li 2 SO 4 Positive Electrode Materials for Bulk‐Type All‐Oxide Solid‐State Batteries
journal, February 2019
- Nagao, Kenji; Sakuda, Atsushi; Hayashi, Akitoshi
- Advanced Materials Interfaces, Vol. 6, Issue 8
Simultaneously Dual Modification of Ni‐Rich Layered Oxide Cathode for High‐Energy Lithium‐Ion Batteries
journal, February 2019
- Yang, Huiping; Wu, Hong‐Hui; Ge, Mingyuan
- Advanced Functional Materials, Vol. 29, Issue 13
High‐Voltage Performance of Ni‐Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation
journal, August 2019
- David, Lamuel; Mohanty, Debasish; Geng, Linxiao
- ChemElectroChem, Vol. 6, Issue 22
Benign Solvation Effect on Electrochemical Intercalation of Triethylmethyl Ammonium into Graphite from Propylene Carbonate
journal, January 2018
- Li, Jiayu; Huang, Yuhao; Wang, Hongyu
- Journal of The Electrochemical Society, Vol. 165, Issue 16
In‐Depth TEM Investigation on Structural Inhomogeneity within a Primary Li x Ni 0.835 Co 0.15 Al 0.015 O 2 Particle: Origin of Capacity Decay during High‐Rate Discharge
journal, November 2019
- Lee, Hyesu; Jo, Eunmi; Chung, Kyung Yoon
- Angewandte Chemie, Vol. 132, Issue 6
Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries
text, January 2020
- Teichert, Philipp; Eshetu, Gebrekidan Gebresilassie; Jahnke, Hannes
- RWTH Aachen University
In-Operando Impedance Spectroscopy and Ultrasonic Measurements during High-Temperature Abuse Experiments on Lithium-Ion Batteries
journal, April 2020
- Zappen, Hendrik; Fuchs, Georg; Gitis, Alexander
- Batteries, Vol. 6, Issue 2
Chemical, Structural, and Electronic Aspects of Formation and Degradation Behavior on Different Length Scales of Ni‐Rich NCM and Li‐Rich HE‐NCM Cathode Materials in Li‐Ion Batteries
text, January 2019
- De Biasi, Lea; Schwarz, Björn; Brezesinski, Torsten
- Karlsruhe
Towards Ultra Low Cobalt Cathodes: A High Fidelity Computational Phase Search of Layered Li-Ni-Mn-Co Oxides
text, January 2018
- Houchins, Gregory; Viswanathan, Venkatasubramanian
- arXiv
Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode
journal, June 2018
- Yan, Pengfei; Zheng, Jianming; Chen, Tianwu
- Nature Communications, Vol. 9, Issue 1