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

Journal Article · Fri Aug 16 00:00:00 EDT 2019 · ChemElectroChem

DOI:https://doi.org/10.1002/celc.201901338· OSTI ID:1561675

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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)

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.

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

Sponsoring Organization:: 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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1561675

Alternate ID(s):: OSTI ID: 1558680

Journal Information:: ChemElectroChem, Vol. 6, Issue 22; ISSN 2196-0216

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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

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

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