Promoting Granular Lithium Sulfide Growth by Soft Acidic-Hard Basic Ionomer Binder for Lithium-Sulfur Batteries

Hyunseok Moon; Myeong Hwa Ryou; Anseong Park; Bo Quan Li; Ha Neul Kim; Namjun Park; Eunbyoul Lee; Kyung Yoon Chung; Jia Qi Huang; Taeeun Yim; Won Bo Lee; Sang Young Lee

doi:10.1021/acsenergylett.4c03522

Promoting Granular Lithium Sulfide Growth by Soft Acidic-Hard Basic Ionomer Binder for Lithium-Sulfur Batteries

Hyunseok Moon, Myeong Hwa Ryou, Anseong Park, Bo Quan Li, Ha Neul Kim, Namjun Park, Eunbyoul Lee, Kyung Yoon Chung, Jia Qi Huang^*, Taeeun Yim^*, Won Bo Lee^*, Sang Young Lee^*

^*Corresponding author for this work

Advanced Research Institute of Multidisciplinary Science

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

Abstract

Electrode passivation limits the reversibility of lithium-sulfur (Li-S) batteries. Pivoting from the prevailing approaches that focus on electrode active materials and electrolytes, herein, we introduce a class of S electrode binders based on soft acidic-hard basic (SAHB) ionomers. The SAHB binder contains a soft cation (tetraallyl ammonium ion, TA⁺) paired with a hard counteranion (nitrate, NO₃^-), allowing matched interactions with Li polysulfides (LiPS) via soft acid-soft base (TA⁺-S_x^2-) and hard base-hard acid (NO₃^--Li⁺) pairings. This intermolecular coupling retards LiPS diffusion, promoting three-dimensional granular Li sulfide (Li₂S) growth, guided by a high Damköhler number (Da). Consequently, the SAHB binder enables a Li-S cell to achieve a high specific capacity of 1545 mAh g_sulfur^-1 (corresponding to 92.3% S utilization) and stable capacity retention (71.5% after 300 cycles at a current density of 1 C), outperforming previously reported S electrode binders.

Original language	English
Pages (from-to)	1654-1663
Number of pages	10
Journal	ACS Energy Letters
Volume	10
Issue number	4
DOIs	https://doi.org/10.1021/acsenergylett.4c03522
Publication status	Published - 11 Apr 2025

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@article{d88355cd19d849579a5b0805dab94c33,

title = "Promoting Granular Lithium Sulfide Growth by Soft Acidic-Hard Basic Ionomer Binder for Lithium-Sulfur Batteries",

abstract = "Electrode passivation limits the reversibility of lithium-sulfur (Li-S) batteries. Pivoting from the prevailing approaches that focus on electrode active materials and electrolytes, herein, we introduce a class of S electrode binders based on soft acidic-hard basic (SAHB) ionomers. The SAHB binder contains a soft cation (tetraallyl ammonium ion, TA+) paired with a hard counteranion (nitrate, NO3-), allowing matched interactions with Li polysulfides (LiPS) via soft acid-soft base (TA+-Sx2-) and hard base-hard acid (NO3--Li+) pairings. This intermolecular coupling retards LiPS diffusion, promoting three-dimensional granular Li sulfide (Li2S) growth, guided by a high Damk{\"o}hler number (Da). Consequently, the SAHB binder enables a Li-S cell to achieve a high specific capacity of 1545 mAh gsulfur-1 (corresponding to 92.3% S utilization) and stable capacity retention (71.5% after 300 cycles at a current density of 1 C), outperforming previously reported S electrode binders.",

author = "Hyunseok Moon and Ryou, {Myeong Hwa} and Anseong Park and Li, {Bo Quan} and Kim, {Ha Neul} and Namjun Park and Eunbyoul Lee and Chung, {Kyung Yoon} and Huang, {Jia Qi} and Taeeun Yim and Lee, {Won Bo} and Lee, {Sang Young}",

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doi = "10.1021/acsenergylett.4c03522",

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T1 - Promoting Granular Lithium Sulfide Growth by Soft Acidic-Hard Basic Ionomer Binder for Lithium-Sulfur Batteries

AU - Moon, Hyunseok

AU - Ryou, Myeong Hwa

AU - Park, Anseong

AU - Li, Bo Quan

AU - Kim, Ha Neul

AU - Park, Namjun

AU - Lee, Eunbyoul

AU - Chung, Kyung Yoon

AU - Huang, Jia Qi

AU - Yim, Taeeun

AU - Lee, Won Bo

AU - Lee, Sang Young

PY - 2025/4/11

Y1 - 2025/4/11

N2 - Electrode passivation limits the reversibility of lithium-sulfur (Li-S) batteries. Pivoting from the prevailing approaches that focus on electrode active materials and electrolytes, herein, we introduce a class of S electrode binders based on soft acidic-hard basic (SAHB) ionomers. The SAHB binder contains a soft cation (tetraallyl ammonium ion, TA+) paired with a hard counteranion (nitrate, NO3-), allowing matched interactions with Li polysulfides (LiPS) via soft acid-soft base (TA+-Sx2-) and hard base-hard acid (NO3--Li+) pairings. This intermolecular coupling retards LiPS diffusion, promoting three-dimensional granular Li sulfide (Li2S) growth, guided by a high Damköhler number (Da). Consequently, the SAHB binder enables a Li-S cell to achieve a high specific capacity of 1545 mAh gsulfur-1 (corresponding to 92.3% S utilization) and stable capacity retention (71.5% after 300 cycles at a current density of 1 C), outperforming previously reported S electrode binders.

AB - Electrode passivation limits the reversibility of lithium-sulfur (Li-S) batteries. Pivoting from the prevailing approaches that focus on electrode active materials and electrolytes, herein, we introduce a class of S electrode binders based on soft acidic-hard basic (SAHB) ionomers. The SAHB binder contains a soft cation (tetraallyl ammonium ion, TA+) paired with a hard counteranion (nitrate, NO3-), allowing matched interactions with Li polysulfides (LiPS) via soft acid-soft base (TA+-Sx2-) and hard base-hard acid (NO3--Li+) pairings. This intermolecular coupling retards LiPS diffusion, promoting three-dimensional granular Li sulfide (Li2S) growth, guided by a high Damköhler number (Da). Consequently, the SAHB binder enables a Li-S cell to achieve a high specific capacity of 1545 mAh gsulfur-1 (corresponding to 92.3% S utilization) and stable capacity retention (71.5% after 300 cycles at a current density of 1 C), outperforming previously reported S electrode binders.

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DO - 10.1021/acsenergylett.4c03522

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JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 4

ER -

Promoting Granular Lithium Sulfide Growth by Soft Acidic-Hard Basic Ionomer Binder for Lithium-Sulfur Batteries

Abstract

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