High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode

Ju Myung Kim; Mark H. Engelhard; Bingyu Lu; Yaobin Xu; Sha Tan; Bethany E. Matthews; Shalini Tripathi; Xia Cao; Chaojiang Niu; Enyuan Hu; Seong Min Bak; Chongmin Wang; Ying Shirley Meng; Ji Guang Zhang; Wu Xu

doi:10.1002/adfm.202207172

High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode

Ju Myung Kim, Mark H. Engelhard, Bingyu Lu, Yaobin Xu, Sha Tan, Bethany E. Matthews, Shalini Tripathi, Xia Cao, Chaojiang Niu, Enyuan Hu, Seong Min Bak, Chongmin Wang, Ying Shirley Meng, Ji Guang Zhang, Wu Xu

Department of Materials Science and Engineering

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

Abstract

The practical application of lithium (Li) metal anode (LMA) is still hindered by non-uniformity of solid electrolyte interphase (SEI), formation of “dead” Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, a facile protection strategy is reported for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)-based bottom layer that is highly stable with LMA and promotes uniform ion flux, and a cross-linked polymer-based top layer that prevents solvation of PEO layer in electrolytes. Li deposited on DL-coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li₂O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi_0.6Mn_0.2Co_0.2O₂ cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm^–2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm^–2 (1.5 C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy-density Li metal batteries.

Original language	English
Article number	2207172
Journal	Advanced Functional Materials
Volume	32
Issue number	48
DOIs	https://doi.org/10.1002/adfm.202207172
Publication status	Published - 2022 Nov 24

Bibliographical note

Funding Information:
This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE-AC05-76RL01830 for Pacific Northwest National Laboratory (PNNL) and the contract no. DE-SC0012704 for Brookhaven National Laboratory (BNL). The XPS measurement was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund. The microscopic and spectroscopic characterizations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. Cryo-FIB/SEM was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS-1542148). PNNL is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. This research used beamline 8-BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract No. DE-SC0012704. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd.

Funding Information:
This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE‐AC05‐76RL01830 for Pacific Northwest National Laboratory (PNNL) and the contract no. DE‐SC0012704 for Brookhaven National Laboratory (BNL). The XPS measurement was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund. The microscopic and spectroscopic characterizations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. Cryo‐FIB/SEM was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS‐1542148). PNNL is operated by Battelle for the DOE under Contract DE‐AC05‐76RL01830. This research used beamline 8‐BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract No. DE‐SC0012704. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd.

Publisher Copyright:
© 2022 Battelle Memorial Institute and The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Materials Science(all)
Condensed Matter Physics

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10.1002/adfm.202207172

Cite this

Kim, J. M., Engelhard, M. H., Lu, B., Xu, Y., Tan, S., Matthews, B. E., Tripathi, S., Cao, X., Niu, C., Hu, E., Bak, S. M., Wang, C., Meng, Y. S., Zhang, J. G., & Xu, W. (2022). High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode. Advanced Functional Materials, 32(48), [2207172]. https://doi.org/10.1002/adfm.202207172

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title = "High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode",

abstract = "The practical application of lithium (Li) metal anode (LMA) is still hindered by non-uniformity of solid electrolyte interphase (SEI), formation of “dead” Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, a facile protection strategy is reported for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)-based bottom layer that is highly stable with LMA and promotes uniform ion flux, and a cross-linked polymer-based top layer that prevents solvation of PEO layer in electrolytes. Li deposited on DL-coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li2O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi0.6Mn0.2Co0.2O2 cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm–2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm–2 (1.5 C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy-density Li metal batteries.",

author = "Kim, {Ju Myung} and Engelhard, {Mark H.} and Bingyu Lu and Yaobin Xu and Sha Tan and Matthews, {Bethany E.} and Shalini Tripathi and Xia Cao and Chaojiang Niu and Enyuan Hu and Bak, {Seong Min} and Chongmin Wang and Meng, {Ying Shirley} and Zhang, {Ji Guang} and Wu Xu",

note = "Funding Information: This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE-AC05-76RL01830 for Pacific Northwest National Laboratory (PNNL) and the contract no. DE-SC0012704 for Brookhaven National Laboratory (BNL). The XPS measurement was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund. The microscopic and spectroscopic characterizations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. Cryo-FIB/SEM was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS-1542148). PNNL is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. This research used beamline 8-BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract No. DE-SC0012704. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd. Funding Information: This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE‐AC05‐76RL01830 for Pacific Northwest National Laboratory (PNNL) and the contract no. DE‐SC0012704 for Brookhaven National Laboratory (BNL). The XPS measurement was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund. The microscopic and spectroscopic characterizations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. Cryo‐FIB/SEM was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS‐1542148). PNNL is operated by Battelle for the DOE under Contract DE‐AC05‐76RL01830. This research used beamline 8‐BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract No. DE‐SC0012704. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd. Publisher Copyright: {\textcopyright} 2022 Battelle Memorial Institute and The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.",

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doi = "10.1002/adfm.202207172",

language = "English",

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T1 - High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode

AU - Kim, Ju Myung

AU - Engelhard, Mark H.

AU - Lu, Bingyu

AU - Xu, Yaobin

AU - Tan, Sha

AU - Matthews, Bethany E.

AU - Tripathi, Shalini

AU - Cao, Xia

AU - Niu, Chaojiang

AU - Hu, Enyuan

AU - Bak, Seong Min

AU - Wang, Chongmin

AU - Meng, Ying Shirley

AU - Zhang, Ji Guang

AU - Xu, Wu

N1 - Funding Information: This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE-AC05-76RL01830 for Pacific Northwest National Laboratory (PNNL) and the contract no. DE-SC0012704 for Brookhaven National Laboratory (BNL). The XPS measurement was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund. The microscopic and spectroscopic characterizations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. Cryo-FIB/SEM was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS-1542148). PNNL is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. This research used beamline 8-BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract No. DE-SC0012704. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd. Funding Information: This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE‐AC05‐76RL01830 for Pacific Northwest National Laboratory (PNNL) and the contract no. DE‐SC0012704 for Brookhaven National Laboratory (BNL). The XPS measurement was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund. The microscopic and spectroscopic characterizations were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE's Office of Biological and Environmental Research and located at PNNL. Cryo‐FIB/SEM was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS‐1542148). PNNL is operated by Battelle for the DOE under Contract DE‐AC05‐76RL01830. This research used beamline 8‐BM (TES) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract No. DE‐SC0012704. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd. Publisher Copyright: © 2022 Battelle Memorial Institute and The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.

PY - 2022/11/24

Y1 - 2022/11/24

N2 - The practical application of lithium (Li) metal anode (LMA) is still hindered by non-uniformity of solid electrolyte interphase (SEI), formation of “dead” Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, a facile protection strategy is reported for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)-based bottom layer that is highly stable with LMA and promotes uniform ion flux, and a cross-linked polymer-based top layer that prevents solvation of PEO layer in electrolytes. Li deposited on DL-coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li2O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi0.6Mn0.2Co0.2O2 cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm–2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm–2 (1.5 C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy-density Li metal batteries.

AB - The practical application of lithium (Li) metal anode (LMA) is still hindered by non-uniformity of solid electrolyte interphase (SEI), formation of “dead” Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, a facile protection strategy is reported for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)-based bottom layer that is highly stable with LMA and promotes uniform ion flux, and a cross-linked polymer-based top layer that prevents solvation of PEO layer in electrolytes. Li deposited on DL-coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li2O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi0.6Mn0.2Co0.2O2 cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm–2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm–2 (1.5 C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy-density Li metal batteries.

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High Current-Density-Charging Lithium Metal Batteries Enabled by Double-Layer Protected Lithium Metal Anode

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