Dual Passivation of Cathode and Anode through Electrode-Electrolyte Interface Engineering Enables Long-Lifespan Li Metal-SPAN Batteries

Yubin He; Peichao Zou; Seong Min Bak; Chunyang Wang; Rui Zhang; Libing Yao; Yonghua Du; Enyuan Hu; Ruoqian Lin; Huolin L. Xin

doi:10.1021/acsenergylett.2c01093

Dual Passivation of Cathode and Anode through Electrode-Electrolyte Interface Engineering Enables Long-Lifespan Li Metal-SPAN Batteries

Yubin He, Peichao Zou, Seong Min Bak, Chunyang Wang, Rui Zhang, Libing Yao, Yonghua Du, Enyuan Hu, Ruoqian Lin, Huolin L. Xin

Department of Materials Science and Engineering

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

9 Citations (Scopus)

Abstract

The reliability and durability of lithium metal (Li⁰)-sulfur batteries are largely limited by the undesired Li⁰plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. Herein, we report the stable operation of a Li⁰-SPAN (sulfurized polyacrylonitrile) battery via an anode-cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li₃N-forming additive (TMS-N₃), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li⁰anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li⁰plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li₂S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/gSPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode-electrolyte interphase engineering strategy has tackled the major limitations of Li-S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from -10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li⁰-S batteries.

Original language	English
Pages (from-to)	2866-2875
Number of pages	10
Journal	ACS Energy Letters
Volume	7
Issue number	9
DOIs	https://doi.org/10.1021/acsenergylett.2c01093
Publication status	Published - 2022 Sept 9

Bibliographical note

Funding Information:
We at the UCI acknowledge support from the Office of Basic Energy Sciences of the U.S. Department of Energy (DOE), under award no. DE-SC0021204 (for TEM studies) and the startup funding of H.L.X. provided by UC Irvine (for electrochemistry and X-ray studies). The authors acknowledge the use of facilities and instrumentation at the UC Irvine Materials Research Institute (IMRI), which is supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center (DMR-2011967). XPS work was performed using instrumentation funded in part by the National Science Foundation Major Research Instrumentation Program under grant no. CHE-1338173. R.L. and E.H. are 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 under contract DE-SC0012704. This research used resources of the 8-BM beamline of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704.

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

All Science Journal Classification (ASJC) codes

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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10.1021/acsenergylett.2c01093

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title = "Dual Passivation of Cathode and Anode through Electrode-Electrolyte Interface Engineering Enables Long-Lifespan Li Metal-SPAN Batteries",

abstract = "The reliability and durability of lithium metal (Li0)-sulfur batteries are largely limited by the undesired Li0plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. Herein, we report the stable operation of a Li0-SPAN (sulfurized polyacrylonitrile) battery via an anode-cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li3N-forming additive (TMS-N3), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li0anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li0plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li2S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/gSPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode-electrolyte interphase engineering strategy has tackled the major limitations of Li-S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from -10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li0-S batteries.",

author = "Yubin He and Peichao Zou and Bak, {Seong Min} and Chunyang Wang and Rui Zhang and Libing Yao and Yonghua Du and Enyuan Hu and Ruoqian Lin and Xin, {Huolin L.}",

note = "Funding Information: We at the UCI acknowledge support from the Office of Basic Energy Sciences of the U.S. Department of Energy (DOE), under award no. DE-SC0021204 (for TEM studies) and the startup funding of H.L.X. provided by UC Irvine (for electrochemistry and X-ray studies). The authors acknowledge the use of facilities and instrumentation at the UC Irvine Materials Research Institute (IMRI), which is supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center (DMR-2011967). XPS work was performed using instrumentation funded in part by the National Science Foundation Major Research Instrumentation Program under grant no. CHE-1338173. R.L. and E.H. are 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 under contract DE-SC0012704. This research used resources of the 8-BM beamline of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = sep,

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doi = "10.1021/acsenergylett.2c01093",

language = "English",

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T1 - Dual Passivation of Cathode and Anode through Electrode-Electrolyte Interface Engineering Enables Long-Lifespan Li Metal-SPAN Batteries

AU - He, Yubin

AU - Zou, Peichao

AU - Bak, Seong Min

AU - Wang, Chunyang

AU - Zhang, Rui

AU - Yao, Libing

AU - Du, Yonghua

AU - Hu, Enyuan

AU - Lin, Ruoqian

AU - Xin, Huolin L.

N1 - Funding Information: We at the UCI acknowledge support from the Office of Basic Energy Sciences of the U.S. Department of Energy (DOE), under award no. DE-SC0021204 (for TEM studies) and the startup funding of H.L.X. provided by UC Irvine (for electrochemistry and X-ray studies). The authors acknowledge the use of facilities and instrumentation at the UC Irvine Materials Research Institute (IMRI), which is supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center (DMR-2011967). XPS work was performed using instrumentation funded in part by the National Science Foundation Major Research Instrumentation Program under grant no. CHE-1338173. R.L. and E.H. are 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 under contract DE-SC0012704. This research used resources of the 8-BM beamline of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/9/9

Y1 - 2022/9/9

N2 - The reliability and durability of lithium metal (Li0)-sulfur batteries are largely limited by the undesired Li0plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. Herein, we report the stable operation of a Li0-SPAN (sulfurized polyacrylonitrile) battery via an anode-cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li3N-forming additive (TMS-N3), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li0anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li0plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li2S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/gSPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode-electrolyte interphase engineering strategy has tackled the major limitations of Li-S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from -10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li0-S batteries.

AB - The reliability and durability of lithium metal (Li0)-sulfur batteries are largely limited by the undesired Li0plating-stripping irreversibility and the detrimental polysulfide dissolution, yet approaches that can simultaneously address the above anodic and cathodic problems are scarce. Herein, we report the stable operation of a Li0-SPAN (sulfurized polyacrylonitrile) battery via an anode-cathode dual-passivation approach. By combination of a fluorinated localized high concentration electrolyte (LHCE) and a Li3N-forming additive (TMS-N3), robust and highly conductive electrode passivation layers are formed in situ on the surface of both the Li0anode and the SPAN cathode. The resulting highly reversible, dendrite-free, and high-density Li0plating morphology enables a high Coulombic efficiency of 99.4%. Advanced tender energy X-ray spectroscopy also reveals the eliminated Li2S formation and minimized polysulfide dissolution in SPAN cathodes, leading to a high capacity of 580 mAh/gSPAN and stable cycling with negligible capacity decay (0.7%) for 800 cycles. This electrode-electrolyte interphase engineering strategy has tackled the major limitations of Li-S batteries in both ether- and carbonate-based electrolyte systems and under a wide temperature range from -10 to +50 °C, thus providing insightful guidelines for the rational design of highly durable and high-energy-density Li0-S batteries.

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Dual Passivation of Cathode and Anode through Electrode-Electrolyte Interface Engineering Enables Long-Lifespan Li Metal-SPAN Batteries

Abstract

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