Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes

Zulipiya Shadike; Hongkyung Lee; Oleg Borodin; Xia Cao; Xiulin Fan; Xuelong Wang; Ruoqian Lin; Seong Min Bak; Sanjit Ghose; Kang Xu; Chunsheng Wang; Jun Liu; Jie Xiao; Xiao Qing Yang; Enyuan Hu

doi:10.1038/s41565-020-00845-5

Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes

Zulipiya Shadike, Hongkyung Lee, Oleg Borodin, Xia Cao, Xiulin Fan, Xuelong Wang, Ruoqian Lin, Seong Min Bak, Sanjit Ghose, Kang Xu, Chunsheng Wang, Jun Liu, Jie Xiao, Xiao Qing Yang, Enyuan Hu

Department of Materials Science and Engineering

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

85 Citations (Scopus)

Abstract

A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li⁺ transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.

Original language	English
Pages (from-to)	549-554
Number of pages	6
Journal	Nature Nanotechnology
Volume	16
Issue number	5
DOIs	https://doi.org/10.1038/s41565-020-00845-5
Publication status	Published - 2021 May

Bibliographical note

Funding Information:
The work done at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract no. DE-SC0012704. The work done at Pacific Northwest National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) under contract no. DE-AC02-05CH11231. The work at the Army Research Laboratory was performed under JCESR, an Energy Research Hub funded by Basic Energy Sciences, US DOE. This research used beamline 28-ID-2 of the National Synchrotron Light Source II, a US DOE Office of Science user facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704.

Publisher Copyright:
© 2021, The Author(s), under exclusive licence to Springer Nature Limited.

All Science Journal Classification (ASJC) codes

Bioengineering
Atomic and Molecular Physics, and Optics
Biomedical Engineering
Materials Science(all)
Condensed Matter Physics
Electrical and Electronic Engineering

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10.1038/s41565-020-00845-5

Cite this

@article{2060ea88d5774acb9fceea2a67c7db10,

title = "Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes",

abstract = "A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li+ transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.",

author = "Zulipiya Shadike and Hongkyung Lee and Oleg Borodin and Xia Cao and Xiulin Fan and Xuelong Wang and Ruoqian Lin and Bak, {Seong Min} and Sanjit Ghose and Kang Xu and Chunsheng Wang and Jun Liu and Jie Xiao and Yang, {Xiao Qing} and Enyuan Hu",

note = "Funding Information: The work done at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract no. DE-SC0012704. The work done at Pacific Northwest National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) under contract no. DE-AC02-05CH11231. The work at the Army Research Laboratory was performed under JCESR, an Energy Research Hub funded by Basic Energy Sciences, US DOE. This research used beamline 28-ID-2 of the National Synchrotron Light Source II, a US DOE Office of Science user facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. Publisher Copyright: {\textcopyright} 2021, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2021",

month = may,

doi = "10.1038/s41565-020-00845-5",

language = "English",

volume = "16",

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AU - Shadike, Zulipiya

AU - Lee, Hongkyung

AU - Borodin, Oleg

AU - Cao, Xia

AU - Fan, Xiulin

AU - Wang, Xuelong

AU - Lin, Ruoqian

AU - Bak, Seong Min

AU - Ghose, Sanjit

AU - Xu, Kang

AU - Wang, Chunsheng

AU - Liu, Jun

AU - Xiao, Jie

AU - Yang, Xiao Qing

AU - Hu, Enyuan

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PY - 2021/5

Y1 - 2021/5

N2 - A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li+ transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.

AB - A comprehensive understanding of the solid–electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes. LiH is identified as a component of the SEI in high abundance, and the possibility of its misidentification as LiF in the literature is discussed. LiF in the SEI is found to have different structural features from LiF in the bulk phase, including a larger lattice parameter and a smaller grain size (<3 nm). These characteristics favour Li+ transport and explain why an ionic insulator, like LiF, has been found to be a favoured component for the SEI. Finally, pair distribution function analysis reveals key amorphous components in the SEI.

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Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes

Abstract

Bibliographical note

All Science Journal Classification (ASJC) codes

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