Effect of the grain arrangements on the thermal stability of polycrystalline nickel-rich lithium-based battery cathodes

Dong Hou; Zhengrui Xu; Zhijie Yang; Chunguang Kuai; Zhijia Du; Cheng Jun Sun; Yang Ren; Jue Liu; Xianghui Xiao; Feng Lin

doi:10.1038/s41467-022-30935-y

Effect of the grain arrangements on the thermal stability of polycrystalline nickel-rich lithium-based battery cathodes

Dong Hou, Zhengrui Xu, Zhijie Yang, Chunguang Kuai, Zhijia Du, Cheng Jun Sun, Yang Ren, Jue Liu, Xianghui Xiao, Feng Lin

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

33 Scopus citations

Abstract

One of the most challenging aspects of developing high-energy lithium-based batteries is the structural and (electro)chemical stability of Ni-rich active cathode materials at thermally-abused and prolonged cell cycling conditions. Here, we report in situ physicochemical characterizations to improve the fundamental understanding of the degradation mechanism of charged polycrystalline Ni-rich cathodes at elevated temperatures (e.g., ≥ 40 °C). Using multiple microscopy, scattering, thermal, and electrochemical probes, we decouple the major contributors for the thermal instability from intertwined factors. Our research work demonstrates that the grain microstructures play an essential role in the thermal stability of polycrystalline lithium-based positive battery electrodes. We also show that the oxygen release, a crucial process during battery thermal runaway, can be regulated by engineering grain arrangements. Furthermore, the grain arrangements can also modulate the macroscopic crystallographic transformation pattern and oxygen diffusion length in layered oxide cathode materials.

Original language	English
Article number	3437
Journal	Nature Communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-022-30935-y
State	Published - Dec 2022

Funding

The work was supported by the National Science Foundation under Grant no. DMR-1832613 (F.L.). This research used beamline 18-ID 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. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. 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. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Some of the NMC materials were produced at the U.S. Department of Energy’s (DOE) CAMP (Cell Analysis, Modeling and Prototyping) Facility, Argonne National Laboratory. The CAMP Facility is fully supported by the DOE Vehicle Technologies Program (VTP) within the core funding of the Applied Battery Research (ABR) for Transportation Program. This work used shared facilities at the Virginia Tech National Center for Earth and Environmental Nanotechnology Infrastructure (NanoEarth), a member of the National Nanotechnology Coordinated Infrastructure (NNCI), supported by NSF (ECCS 1542100 and ECCS 2025151). The authors greatly appreciate the help from Huabin Sun on material synthesis and cell fabrication, and Dr. Yijin Liu on TXM data analysis. The work was supported by the National Science Foundation under Grant no. DMR-1832613 (F.L.). This research used beamline 18-ID 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. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. 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. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Some of the NMC materials were produced at the U.S. Department of Energy’s (DOE) CAMP (Cell Analysis, Modeling and Prototyping) Facility, Argonne National Laboratory. The CAMP Facility is fully supported by the DOE Vehicle Technologies Program (VTP) within the core funding of the Applied Battery Research (ABR) for Transportation Program. This work used shared facilities at the Virginia Tech National Center for Earth and Environmental Nanotechnology Infrastructure (NanoEarth), a member of the National Nanotechnology Coordinated Infrastructure (NNCI), supported by NSF (ECCS 1542100 and ECCS 2025151). The authors greatly appreciate the help from Huabin Sun on material synthesis and cell fabrication, and Dr. Yijin Liu on TXM data analysis.

Funders	Funder number
National Science Foundation	DMR-1832613, ECCS 1542100, ECCS 2025151
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC02-76SF00515
Argonne National Laboratory	DE-AC02-06CH11357
Oak Ridge National Laboratory
Brookhaven National Laboratory	DE-SC0012704
Center for Advanced Materials Processing, Clarkson University

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abstract = "One of the most challenging aspects of developing high-energy lithium-based batteries is the structural and (electro)chemical stability of Ni-rich active cathode materials at thermally-abused and prolonged cell cycling conditions. Here, we report in situ physicochemical characterizations to improve the fundamental understanding of the degradation mechanism of charged polycrystalline Ni-rich cathodes at elevated temperatures (e.g., ≥ 40 °C). Using multiple microscopy, scattering, thermal, and electrochemical probes, we decouple the major contributors for the thermal instability from intertwined factors. Our research work demonstrates that the grain microstructures play an essential role in the thermal stability of polycrystalline lithium-based positive battery electrodes. We also show that the oxygen release, a crucial process during battery thermal runaway, can be regulated by engineering grain arrangements. Furthermore, the grain arrangements can also modulate the macroscopic crystallographic transformation pattern and oxygen diffusion length in layered oxide cathode materials.",

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AU - Hou, Dong

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AU - Yang, Zhijie

AU - Kuai, Chunguang

AU - Du, Zhijia

AU - Sun, Cheng Jun

AU - Ren, Yang

AU - Liu, Jue

AU - Xiao, Xianghui

AU - Lin, Feng

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Effect of the grain arrangements on the thermal stability of polycrystalline nickel-rich lithium-based battery cathodes

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