Lightweight Electrolyte Design for Li/Sulfurized Polyacrylonitrile (SPAN) Batteries

An L. Phan; Bo Nan; Phung M.L. Le; Qiushi Miao; Zhaohui Wu; Kha Le; Fu Chen; Mark Engelhard; Thien Dan Nguyen; Kee Sung Han; Jiyun Heo; Weiran Zhang; Minsung Baek; Jijian Xu; Xiyue Zhang; Ping Liu; Lin Ma; Chunsheng Wang

doi:10.1002/adma.202406594

Lightweight Electrolyte Design for Li/Sulfurized Polyacrylonitrile (SPAN) Batteries

An L. Phan
, Bo Nan
, Phung M.L. Le
, Qiushi Miao
, Zhaohui Wu
, Kha Le
, Fu Chen
, Mark Engelhard
, Thien Dan Nguyen
, Kee Sung Han
, Jiyun Heo
, Weiran Zhang
, Minsung Baek
, Jijian Xu
, Xiyue Zhang
, Ping Liu
, Lin Ma^*
, Chunsheng Wang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

55 Citations (Scopus)

37 Downloads (CityUHK Scholars)

Abstract

Sulfurized polyacrylonitrile (SPAN) recently emerges as a promising cathode for high-energy lithium (Li) metal batteries owing to its high capacity, extended cycle life, and liberty from costly transition metals. As the high capacities of both Li metal and SPAN lead to relatively small electrode weights, the weight and specific energy density of Li/SPAN batteries are particularly sensitive to electrolyte weight, highlighting the importance of minimizing electrolyte density. Besides, the large volume changes of Li metal anode and SPAN cathode require inorganic-rich interphases that can guarantee intactness and protectivity throughout long cycles. This work addresses these crucial aspects with an electrolyte design where lightweight dibutyl ether (DBE) is used as a diluent for concentrated lithium bis(fluorosulfonyl)imide (LiFSI)-triethyl phosphate (TEP) solution. The designed electrolyte (d = 1.04 g mL⁻¹) is 40%–50% lighter than conventional localized high-concentration electrolytes (LHCEs), leading to 12%–20% extra energy density at the cell level. Besides, the use of DBE introduces substantial solvent-diluent affinity, resulting in a unique solvation structure with strengthened capability to form favorable anion-derived inorganic-rich interphases, minimize electrolyte consumption, and improve cell cyclability. The electrolyte also exhibits low volatility and offers good protection to both Li metal anode and SPAN cathode under thermal abuse. © 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

Original language	English
Article number	2406594
Journal	Advanced Materials
Volume	36
Issue number	35
Online published	28 Jun 2024
DOIs	https://doi.org/10.1002/adma.202406594
Publication status	Published - 28 Aug 2024
Externally published	Yes

Funding

A.L.P. and B.N. contributed equally to this work. This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium Phase 2) under DOE contract No. DE\u2010AC05\u201076RL01830 from the Pacific Northwest National Laboratory (PNNL). Lin Ma at UNC Charlotte acknowledges the support by the US National Science Foundation Award No. 2301719.

Research Keywords

high energy density
inorganic SEI
Li metal battery
lightweight electrolyte
sulfurized polyacrylonitrile

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This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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title = "Lightweight Electrolyte Design for Li/Sulfurized Polyacrylonitrile (SPAN) Batteries",

abstract = "Sulfurized polyacrylonitrile (SPAN) recently emerges as a promising cathode for high-energy lithium (Li) metal batteries owing to its high capacity, extended cycle life, and liberty from costly transition metals. As the high capacities of both Li metal and SPAN lead to relatively small electrode weights, the weight and specific energy density of Li/SPAN batteries are particularly sensitive to electrolyte weight, highlighting the importance of minimizing electrolyte density. Besides, the large volume changes of Li metal anode and SPAN cathode require inorganic-rich interphases that can guarantee intactness and protectivity throughout long cycles. This work addresses these crucial aspects with an electrolyte design where lightweight dibutyl ether (DBE) is used as a diluent for concentrated lithium bis(fluorosulfonyl)imide (LiFSI)-triethyl phosphate (TEP) solution. The designed electrolyte (d = 1.04 g mL−1) is 40\%–50\% lighter than conventional localized high-concentration electrolytes (LHCEs), leading to 12\%–20\% extra energy density at the cell level. Besides, the use of DBE introduces substantial solvent-diluent affinity, resulting in a unique solvation structure with strengthened capability to form favorable anion-derived inorganic-rich interphases, minimize electrolyte consumption, and improve cell cyclability. The electrolyte also exhibits low volatility and offers good protection to both Li metal anode and SPAN cathode under thermal abuse. {\textcopyright} 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.",

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year = "2024",

month = aug,

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doi = "10.1002/adma.202406594",

language = "English",

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TY - JOUR

T1 - Lightweight Electrolyte Design for Li/Sulfurized Polyacrylonitrile (SPAN) Batteries

AU - Phan, An L.

AU - Nan, Bo

AU - Le, Phung M.L.

AU - Miao, Qiushi

AU - Wu, Zhaohui

AU - Le, Kha

AU - Chen, Fu

AU - Engelhard, Mark

AU - Dan Nguyen, Thien

AU - Han, Kee Sung

AU - Heo, Jiyun

AU - Zhang, Weiran

AU - Baek, Minsung

AU - Xu, Jijian

AU - Zhang, Xiyue

AU - Liu, Ping

AU - Ma, Lin

AU - Wang, Chunsheng

PY - 2024/8/28

Y1 - 2024/8/28

N2 - Sulfurized polyacrylonitrile (SPAN) recently emerges as a promising cathode for high-energy lithium (Li) metal batteries owing to its high capacity, extended cycle life, and liberty from costly transition metals. As the high capacities of both Li metal and SPAN lead to relatively small electrode weights, the weight and specific energy density of Li/SPAN batteries are particularly sensitive to electrolyte weight, highlighting the importance of minimizing electrolyte density. Besides, the large volume changes of Li metal anode and SPAN cathode require inorganic-rich interphases that can guarantee intactness and protectivity throughout long cycles. This work addresses these crucial aspects with an electrolyte design where lightweight dibutyl ether (DBE) is used as a diluent for concentrated lithium bis(fluorosulfonyl)imide (LiFSI)-triethyl phosphate (TEP) solution. The designed electrolyte (d = 1.04 g mL−1) is 40%–50% lighter than conventional localized high-concentration electrolytes (LHCEs), leading to 12%–20% extra energy density at the cell level. Besides, the use of DBE introduces substantial solvent-diluent affinity, resulting in a unique solvation structure with strengthened capability to form favorable anion-derived inorganic-rich interphases, minimize electrolyte consumption, and improve cell cyclability. The electrolyte also exhibits low volatility and offers good protection to both Li metal anode and SPAN cathode under thermal abuse. © 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

AB - Sulfurized polyacrylonitrile (SPAN) recently emerges as a promising cathode for high-energy lithium (Li) metal batteries owing to its high capacity, extended cycle life, and liberty from costly transition metals. As the high capacities of both Li metal and SPAN lead to relatively small electrode weights, the weight and specific energy density of Li/SPAN batteries are particularly sensitive to electrolyte weight, highlighting the importance of minimizing electrolyte density. Besides, the large volume changes of Li metal anode and SPAN cathode require inorganic-rich interphases that can guarantee intactness and protectivity throughout long cycles. This work addresses these crucial aspects with an electrolyte design where lightweight dibutyl ether (DBE) is used as a diluent for concentrated lithium bis(fluorosulfonyl)imide (LiFSI)-triethyl phosphate (TEP) solution. The designed electrolyte (d = 1.04 g mL−1) is 40%–50% lighter than conventional localized high-concentration electrolytes (LHCEs), leading to 12%–20% extra energy density at the cell level. Besides, the use of DBE introduces substantial solvent-diluent affinity, resulting in a unique solvation structure with strengthened capability to form favorable anion-derived inorganic-rich interphases, minimize electrolyte consumption, and improve cell cyclability. The electrolyte also exhibits low volatility and offers good protection to both Li metal anode and SPAN cathode under thermal abuse. © 2024 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

KW - high energy density

KW - inorganic SEI

KW - Li metal battery

KW - lightweight electrolyte

KW - sulfurized polyacrylonitrile

UR - https://www.scopus.com/pages/publications/85197378518

UR - https://www.scopus.com/pages/publications/85197378518#tab=impact

U2 - 10.1002/adma.202406594

DO - 10.1002/adma.202406594

M3 - RGC 21 - Publication in refereed journal

AN - SCOPUS:85197378518

SN - 0935-9648

VL - 36

JO - Advanced Materials

JF - Advanced Materials

IS - 35

M1 - 2406594

ER -

Lightweight Electrolyte Design for Li/Sulfurized Polyacrylonitrile (SPAN) Batteries

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Research Keywords

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