High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia: Improved Capacity and Mean Voltage Stability during Cycling

Evan M. Erickson; Hadar Sclar; Florian Schipper; Jing Liu; Ruiyuan Tian; Chandan Ghanty; Larisa Burstein; Nicole Leifer; Judith Grinblat; Michael Talianker; Ji Yong Shin; Jordan K. Lampert; Boris Markovsky; Anatoly I. Frenkel; Doron Aurbach

doi:10.1002/aenm.201700708

High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia: Improved Capacity and Mean Voltage Stability during Cycling

Evan M. Erickson, Hadar Sclar, Florian Schipper, Jing Liu, Ruiyuan Tian, Chandan Ghanty, Larisa Burstein, Nicole Leifer, Judith Grinblat, Michael Talianker, Ji Yong Shin, Jordan K. Lampert, Boris Markovsky, Anatoly I. Frenkel, Doron Aurbach

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

159 Scopus citations

Abstract

Li-rich electrode materials of the family xLi₂MnO₃·(1−x)LiNi_aCo_bMn_cO₂ (a + b + c = 1) suffer a voltage fade upon cycling that limits their utilization in commercial batteries despite their extremely high discharge capacity, ≈250 mA h g⁻¹. Li-rich, 0.35Li₂MnO₃·0.65LiNi_0.35Mn_0.45Co_0.20O₂, is exposed to NH₃ at 400 °C, producing materials with improved characteristics: enhanced electrode capacity and a limited average voltage fade during 100 cycles in half cells versus Li. Three main changes caused by NH₃ treatment are established. First, a general bulk reduction of Co and Mn is observed via X-ray photoelectron spectroscopy and X-ray absorption near edge structure. Next, a structural rearrangement lowers the coordination number of CoO and MnO bonds, as well as formation of a surface spinel-like structure. Additionally, Li⁺ removal from the bulk causes the formation of surface LiOH, Li₂CO₃, and Li₂O. These structural and surface changes can enhance the voltage and capacity stability of the Li-rich material electrodes after moderate NH₃ treatment times of 1–2 h.

Original language	English
Journal	Advanced Energy Materials
Volume	7
Issue number	18
DOIs	https://doi.org/10.1002/aenm.201700708
State	Published - 20 Sep 2017

Bibliographical note

Publisher Copyright:
© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Funding

D.A. thanks and acknowledges BASF SE for funding. B.M. thanks Mr. Gregory Avrushenko for his help in maintaining the NH3 gas treatment apparatus and useful discussions. A.I.F. and J.L. acknowledge support by the U.S. National Science Foundation Grant No. CHE-1413937. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

Funders	Funder number
DOE Office of Science
U.S. National Science Foundation	CHE-1413937
U.S. Department of Energy
BASF
Office of Science
Argonne National Laboratory	DE-AC02-06CH11357

Keywords

ammonia treatment
cathodes
lithium-ion batteries
lithium-rich materials
stabilization
voltage fade

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/aenm.201700708

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Erickson, E. M., Sclar, H., Schipper, F., Liu, J., Tian, R., Ghanty, C., Burstein, L., Leifer, N., Grinblat, J., Talianker, M., Shin, J. Y., Lampert, J. K., Markovsky, B., Frenkel, A. I., & Aurbach, D. (2017). High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia: Improved Capacity and Mean Voltage Stability during Cycling. Advanced Energy Materials, 7(18). https://doi.org/10.1002/aenm.201700708

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title = "High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia: Improved Capacity and Mean Voltage Stability during Cycling",

abstract = "Li-rich electrode materials of the family xLi2MnO3·(1−x)LiNiaCobMncO2 (a + b + c = 1) suffer a voltage fade upon cycling that limits their utilization in commercial batteries despite their extremely high discharge capacity, ≈250 mA h g−1. Li-rich, 0.35Li2MnO3·0.65LiNi0.35Mn0.45Co0.20O2, is exposed to NH3 at 400 °C, producing materials with improved characteristics: enhanced electrode capacity and a limited average voltage fade during 100 cycles in half cells versus Li. Three main changes caused by NH3 treatment are established. First, a general bulk reduction of Co and Mn is observed via X-ray photoelectron spectroscopy and X-ray absorption near edge structure. Next, a structural rearrangement lowers the coordination number of CoO and MnO bonds, as well as formation of a surface spinel-like structure. Additionally, Li+ removal from the bulk causes the formation of surface LiOH, Li2CO3, and Li2O. These structural and surface changes can enhance the voltage and capacity stability of the Li-rich material electrodes after moderate NH3 treatment times of 1–2 h.",

keywords = "ammonia treatment, cathodes, lithium-ion batteries, lithium-rich materials, stabilization, voltage fade",

author = "Erickson, {Evan M.} and Hadar Sclar and Florian Schipper and Jing Liu and Ruiyuan Tian and Chandan Ghanty and Larisa Burstein and Nicole Leifer and Judith Grinblat and Michael Talianker and Shin, {Ji Yong} and Lampert, {Jordan K.} and Boris Markovsky and Frenkel, {Anatoly I.} and Doron Aurbach",

note = "Publisher Copyright: {\textcopyright} 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2017",

month = sep,

day = "20",

doi = "10.1002/aenm.201700708",

language = "אנגלית",

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Erickson, EM, Sclar, H, Schipper, F, Liu, J, Tian, R, Ghanty, C, Burstein, L, Leifer, N, Grinblat, J, Talianker, M, Shin, JY, Lampert, JK, Markovsky, B, Frenkel, AI & Aurbach, D 2017, 'High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia: Improved Capacity and Mean Voltage Stability during Cycling', Advanced Energy Materials, vol. 7, no. 18. https://doi.org/10.1002/aenm.201700708

TY - JOUR

T1 - High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia

T2 - Improved Capacity and Mean Voltage Stability during Cycling

AU - Erickson, Evan M.

AU - Sclar, Hadar

AU - Schipper, Florian

AU - Liu, Jing

AU - Tian, Ruiyuan

AU - Ghanty, Chandan

AU - Burstein, Larisa

AU - Leifer, Nicole

AU - Grinblat, Judith

AU - Talianker, Michael

AU - Shin, Ji Yong

AU - Lampert, Jordan K.

AU - Markovsky, Boris

AU - Frenkel, Anatoly I.

AU - Aurbach, Doron

PY - 2017/9/20

Y1 - 2017/9/20

N2 - Li-rich electrode materials of the family xLi2MnO3·(1−x)LiNiaCobMncO2 (a + b + c = 1) suffer a voltage fade upon cycling that limits their utilization in commercial batteries despite their extremely high discharge capacity, ≈250 mA h g−1. Li-rich, 0.35Li2MnO3·0.65LiNi0.35Mn0.45Co0.20O2, is exposed to NH3 at 400 °C, producing materials with improved characteristics: enhanced electrode capacity and a limited average voltage fade during 100 cycles in half cells versus Li. Three main changes caused by NH3 treatment are established. First, a general bulk reduction of Co and Mn is observed via X-ray photoelectron spectroscopy and X-ray absorption near edge structure. Next, a structural rearrangement lowers the coordination number of CoO and MnO bonds, as well as formation of a surface spinel-like structure. Additionally, Li+ removal from the bulk causes the formation of surface LiOH, Li2CO3, and Li2O. These structural and surface changes can enhance the voltage and capacity stability of the Li-rich material electrodes after moderate NH3 treatment times of 1–2 h.

AB - Li-rich electrode materials of the family xLi2MnO3·(1−x)LiNiaCobMncO2 (a + b + c = 1) suffer a voltage fade upon cycling that limits their utilization in commercial batteries despite their extremely high discharge capacity, ≈250 mA h g−1. Li-rich, 0.35Li2MnO3·0.65LiNi0.35Mn0.45Co0.20O2, is exposed to NH3 at 400 °C, producing materials with improved characteristics: enhanced electrode capacity and a limited average voltage fade during 100 cycles in half cells versus Li. Three main changes caused by NH3 treatment are established. First, a general bulk reduction of Co and Mn is observed via X-ray photoelectron spectroscopy and X-ray absorption near edge structure. Next, a structural rearrangement lowers the coordination number of CoO and MnO bonds, as well as formation of a surface spinel-like structure. Additionally, Li+ removal from the bulk causes the formation of surface LiOH, Li2CO3, and Li2O. These structural and surface changes can enhance the voltage and capacity stability of the Li-rich material electrodes after moderate NH3 treatment times of 1–2 h.

KW - ammonia treatment

KW - cathodes

KW - lithium-ion batteries

KW - lithium-rich materials

KW - stabilization

KW - voltage fade

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U2 - 10.1002/aenm.201700708

DO - 10.1002/aenm.201700708

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SN - 1614-6832

VL - 7

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 18

ER -

High-Temperature Treatment of Li-Rich Cathode Materials with Ammonia: Improved Capacity and Mean Voltage Stability during Cycling

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

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