Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials

Ruoqian Lin; Seong Min Bak; Youngho Shin; Rui Zhang; Chunyang Wang; Kim Kisslinger; Mingyuan Ge; Xiaojing Huang; Zulipiya Shadike; Ajith Pattammattel; Hanfei Yan; Yong Chu; Jinpeng Wu; Wanli Yang; M. Stanley Whittingham; Huolin L. Xin; Xiao Qing Yang

doi:10.1038/s41467-021-22635-w

Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials

Ruoqian Lin, Seong Min Bak, Youngho Shin, Rui Zhang, Chunyang Wang, Kim Kisslinger, Mingyuan Ge, Xiaojing Huang, Zulipiya Shadike, Ajith Pattammattel, Hanfei Yan, Yong Chu, Jinpeng Wu, Wanli Yang, M. Stanley Whittingham, Huolin L. Xin, Xiao Qing Yang

Department of Materials Science and Engineering

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

40 Citations (Scopus)

Abstract

High-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials’ thermal and cycling stability. Even though promising, the fundamental mechanism of the nickel concentration gradient’s stabilization effect remains elusive because it is inseparable from nickel’s valence gradient effect. To isolate nickel’s valence gradient effect and understand its fundamental stabilization mechanism, we design and synthesize a LiNi_0.8Mn_0.1Co_0.1O₂ material that is compositionally uniform and has a hierarchical valence gradient. The nickel valence gradient material shows superior cycling and thermal stability than the conventional one. The result suggests creating an oxidation state gradient that hides the more capacitive but less stable Ni³⁺ away from the secondary particle surfaces is a viable principle towards the optimization of high-nickel content cathode materials.

Original language	English
Article number	2350
Journal	Nature communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-22635-w
Publication status	Published - 2021 Dec 1

Bibliographical note

Funding Information:
Dr. Ruoqian Lin, Dr. Seongmin Bak, and Dr. Xiao-Qing Yang were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under Contract DESC0012704. Work done by Dr. Chunyang Wang and Dr. Huolin Xin was supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Award Number: DE-EE0008444 and the startup funding of Huolin Xin. Mr. Rui Zhang was supported by the startup funding of Huolin Xin. Dr. Y. Shin was supported by the Office of Vehicle Technologies of the U. S. Department of Energy under contract number DE-AC02-06CH11357. Dr. S. Whittingham is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract No. DE-EE0007765. This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used resources 3-ID, 18-ID, and 28-ID-2 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Soft X-ray characterization was carried out at the Advanced Light Source (ALS), a US Department of Energy, Office of Science User Facility under Contract No. DE-AC02-05CH11231. The XRD experiments were carried out at Beamline 17-BM-B of the Advanced Photon Source (APS) which is supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Science, under Contract No. DE-AC02-06CH11357.

Publisher Copyright:
© 2021, The Author(s).

All Science Journal Classification (ASJC) codes

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

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Lin, R., Bak, S. M., Shin, Y., Zhang, R., Wang, C., Kisslinger, K., Ge, M., Huang, X., Shadike, Z., Pattammattel, A., Yan, H., Chu, Y., Wu, J., Yang, W., Whittingham, M. S., Xin, H. L., & Yang, X. Q. (2021). Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials. Nature communications, 12(1), [2350]. https://doi.org/10.1038/s41467-021-22635-w

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title = "Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials",

abstract = "High-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials{\textquoteright} thermal and cycling stability. Even though promising, the fundamental mechanism of the nickel concentration gradient{\textquoteright}s stabilization effect remains elusive because it is inseparable from nickel{\textquoteright}s valence gradient effect. To isolate nickel{\textquoteright}s valence gradient effect and understand its fundamental stabilization mechanism, we design and synthesize a LiNi0.8Mn0.1Co0.1O2 material that is compositionally uniform and has a hierarchical valence gradient. The nickel valence gradient material shows superior cycling and thermal stability than the conventional one. The result suggests creating an oxidation state gradient that hides the more capacitive but less stable Ni3+ away from the secondary particle surfaces is a viable principle towards the optimization of high-nickel content cathode materials.",

author = "Ruoqian Lin and Bak, {Seong Min} and Youngho Shin and Rui Zhang and Chunyang Wang and Kim Kisslinger and Mingyuan Ge and Xiaojing Huang and Zulipiya Shadike and Ajith Pattammattel and Hanfei Yan and Yong Chu and Jinpeng Wu and Wanli Yang and Whittingham, {M. Stanley} and Xin, {Huolin L.} and Yang, {Xiao Qing}",

note = "Funding Information: Dr. Ruoqian Lin, Dr. Seongmin Bak, and Dr. Xiao-Qing Yang were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under Contract DESC0012704. Work done by Dr. Chunyang Wang and Dr. Huolin Xin was supported by the U.S. Department of Energy{\textquoteright}s Office of Energy Efficiency and Renewable Energy (EERE) under the Award Number: DE-EE0008444 and the startup funding of Huolin Xin. Mr. Rui Zhang was supported by the startup funding of Huolin Xin. Dr. Y. Shin was supported by the Office of Vehicle Technologies of the U. S. Department of Energy under contract number DE-AC02-06CH11357. Dr. S. Whittingham is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract No. DE-EE0007765. This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used resources 3-ID, 18-ID, and 28-ID-2 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Soft X-ray characterization was carried out at the Advanced Light Source (ALS), a US Department of Energy, Office of Science User Facility under Contract No. DE-AC02-05CH11231. The XRD experiments were carried out at Beamline 17-BM-B of the Advanced Photon Source (APS) which is supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Science, under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2021, The Author(s).",

year = "2021",

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doi = "10.1038/s41467-021-22635-w",

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T1 - Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials

AU - Lin, Ruoqian

AU - Bak, Seong Min

AU - Shin, Youngho

AU - Zhang, Rui

AU - Wang, Chunyang

AU - Kisslinger, Kim

AU - Ge, Mingyuan

AU - Huang, Xiaojing

AU - Shadike, Zulipiya

AU - Pattammattel, Ajith

AU - Yan, Hanfei

AU - Chu, Yong

AU - Wu, Jinpeng

AU - Yang, Wanli

AU - Whittingham, M. Stanley

AU - Xin, Huolin L.

AU - Yang, Xiao Qing

N1 - Funding Information: Dr. Ruoqian Lin, Dr. Seongmin Bak, and Dr. Xiao-Qing Yang were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under Contract DESC0012704. Work done by Dr. Chunyang Wang and Dr. Huolin Xin was supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Award Number: DE-EE0008444 and the startup funding of Huolin Xin. Mr. Rui Zhang was supported by the startup funding of Huolin Xin. Dr. Y. Shin was supported by the Office of Vehicle Technologies of the U. S. Department of Energy under contract number DE-AC02-06CH11357. Dr. S. Whittingham is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract No. DE-EE0007765. This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used resources 3-ID, 18-ID, and 28-ID-2 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Soft X-ray characterization was carried out at the Advanced Light Source (ALS), a US Department of Energy, Office of Science User Facility under Contract No. DE-AC02-05CH11231. The XRD experiments were carried out at Beamline 17-BM-B of the Advanced Photon Source (APS) which is supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Science, under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2021, The Author(s).

PY - 2021/12/1

Y1 - 2021/12/1

N2 - High-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials’ thermal and cycling stability. Even though promising, the fundamental mechanism of the nickel concentration gradient’s stabilization effect remains elusive because it is inseparable from nickel’s valence gradient effect. To isolate nickel’s valence gradient effect and understand its fundamental stabilization mechanism, we design and synthesize a LiNi0.8Mn0.1Co0.1O2 material that is compositionally uniform and has a hierarchical valence gradient. The nickel valence gradient material shows superior cycling and thermal stability than the conventional one. The result suggests creating an oxidation state gradient that hides the more capacitive but less stable Ni3+ away from the secondary particle surfaces is a viable principle towards the optimization of high-nickel content cathode materials.

AB - High-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials’ thermal and cycling stability. Even though promising, the fundamental mechanism of the nickel concentration gradient’s stabilization effect remains elusive because it is inseparable from nickel’s valence gradient effect. To isolate nickel’s valence gradient effect and understand its fundamental stabilization mechanism, we design and synthesize a LiNi0.8Mn0.1Co0.1O2 material that is compositionally uniform and has a hierarchical valence gradient. The nickel valence gradient material shows superior cycling and thermal stability than the conventional one. The result suggests creating an oxidation state gradient that hides the more capacitive but less stable Ni3+ away from the secondary particle surfaces is a viable principle towards the optimization of high-nickel content cathode materials.

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Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials

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