Unveiling the Role of Al2O3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries
Abstract
Recent achievements in high-energy batteries have been made by using Ni-rich NMC cathodes (LiNixMnyCo1–x–yO 2with x > 0.5) in conjunction with higher cell voltages. However, these gains have come at a cost of fast capacity fade and poor rate performace. In our previous study, we showed that Al2O3 ALD coatings on LiNi0.8Mn0.1Co0.1O2 (NMC811) and LiNi0.8Co0.15Al0.05O2 (NCA) cathodes prevented surface phase transitions, reduced impedance, and extended cycle life in high voltage cells. In this work, neutron diffraction (ND), X-ray photoelectron spectroscopy (XPS), and electron energy loss spectroscopy (EELS) are used to fully investigate the mechanism by which ALD surface coatings mitigate NMC811 cathode degredation. Refinement of ND patterns indicated no changes in the bulk crystal structure of cycled cathodes with or without the Al2O3 coating. Rather, the improved performance of ALD-coated cathodes is clearly due to surface stabilization. EELS established that all three transition metal oxidation states were reduced at the surface of the uncoated cathode after cycling, whereas the coated cathode showed no changes in surface oxidation states relative to the bulk. The surface coatings also prevented transition metal dissolution and crossover. XPS analysis of the anode harvested from cycled cells with uncoated cathodes showed significant amounts of Mn depositedmore »
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[1];
[1];
[4]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- XALT Energy, LLC, Midland, MI (United States)
- ForgeNano, LLC, Louisville, CO (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
- OSTI Identifier:
- 1784207
- Grant/Contract Number:
- AC05-00OR22725; EE0005384; NFE-11-03678; TSA 14-587; LS-111201AMMW; SC0010230
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Energy Materials
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 2; Journal ID: ISSN 2574-0962
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Li-ion battery; full concentration gradient; NMC811; ALD coating; electrochemistry; EELS; XPS; neutron diffraction
Citation Formats
David, Lamuel, Dahlberg, Kevin, Mohanty, Debasish, Ruther, Rose E., Huq, Ashfia, Chi, Miaofang, An, Seong Jin, Mao, Chengyu, King, David M., Stevenson, Lisa, and Wood, David L. Unveiling the Role of Al2O3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries. United States: N. p., 2019.
Web. doi:10.1021/acsaem.8b01877.
David, Lamuel, Dahlberg, Kevin, Mohanty, Debasish, Ruther, Rose E., Huq, Ashfia, Chi, Miaofang, An, Seong Jin, Mao, Chengyu, King, David M., Stevenson, Lisa, & Wood, David L. Unveiling the Role of Al2O3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries. United States. https://doi.org/10.1021/acsaem.8b01877
David, Lamuel, Dahlberg, Kevin, Mohanty, Debasish, Ruther, Rose E., Huq, Ashfia, Chi, Miaofang, An, Seong Jin, Mao, Chengyu, King, David M., Stevenson, Lisa, and Wood, David L. Fri .
"Unveiling the Role of Al2O3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries". United States. https://doi.org/10.1021/acsaem.8b01877. https://www.osti.gov/servlets/purl/1784207.
@article{osti_1784207,
title = {Unveiling the Role of Al2O3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries},
author = {David, Lamuel and Dahlberg, Kevin and Mohanty, Debasish and Ruther, Rose E. and Huq, Ashfia and Chi, Miaofang and An, Seong Jin and Mao, Chengyu and King, David M. and Stevenson, Lisa and Wood, David L.},
abstractNote = {Recent achievements in high-energy batteries have been made by using Ni-rich NMC cathodes (LiNixMnyCo1–x–yO 2with x > 0.5) in conjunction with higher cell voltages. However, these gains have come at a cost of fast capacity fade and poor rate performace. In our previous study, we showed that Al2O3 ALD coatings on LiNi0.8Mn0.1Co0.1O2 (NMC811) and LiNi0.8Co0.15Al0.05O2 (NCA) cathodes prevented surface phase transitions, reduced impedance, and extended cycle life in high voltage cells. In this work, neutron diffraction (ND), X-ray photoelectron spectroscopy (XPS), and electron energy loss spectroscopy (EELS) are used to fully investigate the mechanism by which ALD surface coatings mitigate NMC811 cathode degredation. Refinement of ND patterns indicated no changes in the bulk crystal structure of cycled cathodes with or without the Al2O3 coating. Rather, the improved performance of ALD-coated cathodes is clearly due to surface stabilization. EELS established that all three transition metal oxidation states were reduced at the surface of the uncoated cathode after cycling, whereas the coated cathode showed no changes in surface oxidation states relative to the bulk. The surface coatings also prevented transition metal dissolution and crossover. XPS analysis of the anode harvested from cycled cells with uncoated cathodes showed significant amounts of Mn deposited within the SEI. In contrast, no Mn could be detected on the anodes cycled with coated cathodes. These results affirm that ALD coatings can effectively reduce the reactivity of the NMC surface and prevent detrimental side reactions that shorten battery cycle life.},
doi = {10.1021/acsaem.8b01877},
journal = {ACS Applied Energy Materials},
number = 2,
volume = 2,
place = {United States},
year = {Fri Jan 11 00:00:00 EST 2019},
month = {Fri Jan 11 00:00:00 EST 2019}
}
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