High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation

David, Lamuel Abraham; Mohanty, Debasish; Geng, Linxiao; Ruther, Rose E.; Sefat, Athena Safa; Cakmak, Ercan; Veith, Gabriel M.; Meyer, III, Harry M.; Wang, Hsin; Wood, III, David L.

doi:10.1002/celc.201901338

Title: High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation

Abstract

High-voltage Ni-rich cathodes have been studied as a possible way to achieve high energy density in Li-ion batteries. However, capacity fade due to structural changes at high voltages has limited their applications. In this study, we identify 4.5 V (vs. graphite) as the optimum upper cutoff voltage (UCV) for a Ni-rich NCA cathode [LiNi_0.8Co_0.15Al_0.05O₂]. At this UCV, NCA delivers a 12 % increase in reversible capacity (when discharged to 2.5 V) and retains 92 % of its initial capacity after 100 cycles at 1C/-1C cycling when compared to 4.2 V as UCV. By increasing UCV to 4.7 V, the discharge capacity can be raised to >200 mAh/g. However, the rate of capacity fade is greater when compared to 4.5 V as UCV. This increased rate of capacity fade, at higher UCV, is related to irreversible lattice contractions that leads to structural rearrangement at charged states during high-voltage cycling. Lastly, our results show a change in transition metal oxidation states and an onset of structural ordering occurs when the UCV is 4.7 V.

Authors:

^[1];

^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: Fri Aug 16 00:00:00 EDT 2019

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

OSTI Identifier:: 1561675

Alternate Identifier(s):: OSTI ID: 1558680

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: ChemElectroChem

Additional Journal Information:: Journal Volume: 6; Journal Issue: 22; Journal ID: ISSN 2196-0216

Publisher:: ChemPubSoc Europe

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Li-ion battery; Ni-rich cathodes; electrochemistry; magnetic susceptibility; in situ XRD

Citation Formats


                    David, Lamuel Abraham, Mohanty, Debasish, Geng, Linxiao, Ruther, Rose E., Sefat, Athena Safa, Cakmak, Ercan, Veith, Gabriel M., Meyer, III, Harry M., Wang, Hsin, and Wood, III, David L. High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation.  United States: N. p., 2019. 
Web.  doi:10.1002/celc.201901338.

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                    David, Lamuel Abraham, Mohanty, Debasish, Geng, Linxiao, Ruther, Rose E., Sefat, Athena Safa, Cakmak, Ercan, Veith, Gabriel M., Meyer, III, Harry M., Wang, Hsin, & Wood, III, David L. High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation.  United States.  https://doi.org/10.1002/celc.201901338

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                    David, Lamuel Abraham, Mohanty, Debasish, Geng, Linxiao, Ruther, Rose E., Sefat, Athena Safa, Cakmak, Ercan, Veith, Gabriel M., Meyer, III, Harry M., Wang, Hsin, and Wood, III, David L. Fri .  
"High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation".  United States.  https://doi.org/10.1002/celc.201901338.  https://www.osti.gov/servlets/purl/1561675.

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@article{osti_1561675,

  title        = {High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation},

  author       = {David, Lamuel Abraham and Mohanty, Debasish and Geng, Linxiao and Ruther, Rose E. and Sefat, Athena Safa and Cakmak, Ercan and Veith, Gabriel M. and Meyer, III, Harry M. and Wang, Hsin and Wood, III, David L.},

  abstractNote = {High-voltage Ni-rich cathodes have been studied as a possible way to achieve high energy density in Li-ion batteries. However, capacity fade due to structural changes at high voltages has limited their applications. In this study, we identify 4.5 V (vs. graphite) as the optimum upper cutoff voltage (UCV) for a Ni-rich NCA cathode [LiNi0.8Co0.15Al0.05O2]. At this UCV, NCA delivers a 12 % increase in reversible capacity (when discharged to 2.5 V) and retains 92 % of its initial capacity after 100 cycles at 1C/-1C cycling when compared to 4.2 V as UCV. By increasing UCV to 4.7 V, the discharge capacity can be raised to >200 mAh/g. However, the rate of capacity fade is greater when compared to 4.5 V as UCV. This increased rate of capacity fade, at higher UCV, is related to irreversible lattice contractions that leads to structural rearrangement at charged states during high-voltage cycling. Lastly, our results show a change in transition metal oxidation states and an onset of structural ordering occurs when the UCV is 4.7 V.},

  doi          = {10.1002/celc.201901338},

  journal      = {ChemElectroChem},

  number       = 22,

  volume       = 6,

  place        = {United States},

  year         = {Fri Aug 16 00:00:00 EDT 2019},

  month        = {Fri Aug 16 00:00:00 EDT 2019}

}

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Title: High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation

Abstract

Citation Formats

Calendar Aging of NCA Lithium-Ion Batteries Investigated by Differential Voltage Analysis and Coulomb Tracking journal, October 2016

Magnetic properties of LixNiyMnyCo1−2yO2 (0.2≤1−2y≤0.5, 0≤x≤1) journal, April 2012

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Direct Observation of Lattice Aluminum Environments in Li Ion Cathodes LiNi 1– y – z Co y Al z O 2 and Al-Doped LiNi x Mn y Co z O 2 via 27 Al MAS NMR Spectroscopy journal, June 2016

Metal segregation in hierarchically structured cathode materials for high-energy lithium batteries journal, January 2016

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Capacity fading of LiAlyNi1−x−yCoxO2 cathode for lithium-ion batteries during accelerated calendar and cycle life tests (effect of depth of discharge in charge–discharge cycling on the suppression of the micro-crack generation of LiAlyNi1−x−yCoxO2 particle) journal, August 2014

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Structural, magnetic and electrochemical properties of LiNi0.5Mn0.5O2 as positive electrode for Li-ion batteries journal, March 2007

Investigation of the Structural Changes in Li[NiyMnyCo(1−2y)]O2(y = 0.05) upon Electrochemical Lithium Deintercalation journal, February 2010

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Effect of Al 2 O 3 Coating on Stabilizing LiNi 0.4 Mn 0.4 Co 0.2 O 2 Cathodes journal, August 2015

In Situ X-ray Diffraction Study of Layered Li–Ni–Mn–Co Oxides: Effect of Particle Size and Structural Stability of Core–Shell Materials journal, December 2015

Structural transformation of a lithium-rich Li1.2Co0.1Mn0.55Ni0.15O2 cathode during high voltage cycling resolved by in situ X-ray diffraction journal, May 2013

Synthesis and characterization of layer structured solid solutions in the system of LiCoO2–Li2MnO3 journal, February 1999

Staging Phase Transitions in Li[sub x]CoO[sub 2] journal, January 2002

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journal, January 2016

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journal, July 2010

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Use of amine electride chemistry to prepare molybdenum disulfide intercalation compounds
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Capacity fading of LiAlyNi1−x−yCoxO2 cathode for lithium-ion batteries during accelerated calendar and cycle life tests (effect of depth of discharge in charge–discharge cycling on the suppression of the micro-crack generation of LiAlyNi1−x−yCoxO2 particle)
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journal, January 2011

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journal, January 2007

In Charge of the World: Electrochemical Energy Storage
journal, March 2013

Surface changes on LiNi0.8Co0.2O2 particles during testing of high-power lithium-ion cells
journal, August 2002

Thermal Stability of Lithium Nickel Oxide Derivatives. Part I: Li _x Ni _1.02 O ₂ and Li _x Ni _0.89 Al _0.16 O ₂ ( x = 0.50 and 0.30)
journal, November 2003

Effect of Al ₂ O ₃ Coating on Stabilizing LiNi _0.4 Mn _0.4 Co _0.2 O ₂ Cathodes
journal, August 2015

In Situ X-ray Diffraction Study of Layered Li–Ni–Mn–Co Oxides: Effect of Particle Size and Structural Stability of Core–Shell Materials
journal, December 2015

Structural transformation of a lithium-rich Li1.2Co0.1Mn0.55Ni0.15O2 cathode during high voltage cycling resolved by in situ X-ray diffraction
journal, May 2013

Synthesis and characterization of layer structured solid solutions in the system of LiCoO2–Li2MnO3
journal, February 1999

Staging Phase Transitions in Li[sub x]CoO[sub 2]
journal, January 2002

Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi _0.8 Co _0.15 Al _0.05 O ₂ (NCA)
journal, January 2018

Structural transformation in a Li1.2Co0.1Mn0.55Ni0.15O2 lithium-ion battery cathode during high-voltage hold
journal, January 2013

A comparative study on structural changes of LiCo1/3Ni1/3Mn1/3O2 and LiNi0.8Co0.15Al0.05O2 during first charge using in situ XRD
journal, August 2006

Resolving the degradation pathways in high-voltage oxides for high-energy-density lithium-ion batteries; Alternation in chemistry, composition and crystal structures
journal, June 2017

Correlating Structural Changes and Gas Evolution during the Thermal Decomposition of Charged Li _x Ni _0.8 Co _0.15 Al _0.05 O ₂ Cathode Materials
journal, January 2013

Structural Origin of Overcharge-Induced Thermal Instability of Ni-Containing Layered-Cathodes for High-Energy-Density Lithium Batteries
journal, September 2011

Driving change in the battery industry
journal, May 2014

Prospects for reducing the processing cost of lithium ion batteries
journal, February 2015

Structural Changes and Thermal Stability of Charged LiNi _x Mn _y Co _z O ₂ Cathode Materials Studied by Combined In Situ Time-Resolved XRD and Mass Spectroscopy
journal, December 2014