Implanting single-atom N2-Fe-B2 catalytic sites in carbon hosts to stabilize high-loading and lean-electrolyte lithium-sulfur batteries

Sha Li; Jiande Lin; Bin Chang; Daiwen Yang; De Yin Wu; Junhao Wang; Weijia Zhou; Hong Liu; Shuhui Sun; Li Zhang

doi:10.1016/j.ensm.2022.11.045

Implanting single-atom N₂-Fe-B₂ catalytic sites in carbon hosts to stabilize high-loading and lean-electrolyte lithium-sulfur batteries

Sha Li, Jiande Lin, Bin Chang^*, Daiwen Yang, De Yin Wu^*, Junhao Wang, Weijia Zhou, Hong Liu, Shuhui Sun, Li Zhang

^*Corresponding author for this work

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

50 Scopus citations

Abstract

Lithium-sulfur (Li-S) batteries suffer from soluble lithium polysulfide (LiPS) shuttling and sluggish redox kinetics. The rational design of carbon-supported single-atom catalysts (SACs) as both LiPS immobilizers and sulfur redox promoters is of great significance for high-loading and lean-electrolyte Li-S batteries. However, the most popular nonpolar porphyrin-like transition metal-nitrogen (M-N₄) SACs cannot maximize the catalytic activity of the metal center. Herein, a B, N co-coordinated N₂-Fe-B₂ SAC embedded in a B, N-rich carbon matrix (denoted as Fe SAs@BCN) is disclosed for the first time to construct state-of-the-art Li-S batteries. We reveal experimentally and theoretically that the asymmetric N₂-Fe-B₂ configuration not only rapidly captures LiPSs through strong Lewis acid-base interactions, but also greatly catalyzes the bidirectional sulfur redox chemistry by lowering the Li₂S deposition/decomposition energy barriers. As such, the well-designed SACs enable Li-S batteries to promise extraordinary durability (82% retention over 1000 cycles at 5 C) and high areal capacities even under harsh sulfur mass loadings. More encouragingly, a 359 Wh kg⁻¹ pouch cell with an ultrahigh loading of 11.6 mg·_S cm⁻² and a lean electrolyte to sulfur (E/S) ratio of 3 µL mg·_S⁻¹ is further demonstrated. This work shows that N₂-Fe-B₂ SACs hold great promise in realizing high-energy-density Li-S batteries.

Original language	English (US)
Pages (from-to)	94-104
Number of pages	11
Journal	Energy Storage Materials
Volume	55
DOIs	https://doi.org/10.1016/j.ensm.2022.11.045
State	Published - Jan 2023

Bibliographical note

Funding Information:
The authors acknowledge financial support from the National Natural Science Foundation of China (NSFC, 21875155 , 22032004 , 51972147 , 52022037 , and 52202366 ), the support of the National Key Research and Development Program of China ( 2021YFA1201502 ), the support of Nanqiang Young Top-notch Talent Fellowship in Xiamen University, Taishan Scholars Project Special Funds ( tsqn201812083 ), and the Natural Sciences and Engineering Research Council of Canada (NSERC).

Publisher Copyright:
© 2022 Elsevier B.V.

Keywords

Bidirectional sulfur redox
High-energy-density
Lithium-sulfur batteries
N-Fe-B configuration
Single atom catalysts

ASJC Scopus subject areas

Renewable Energy, Sustainability and the Environment
General Materials Science
Energy Engineering and Power Technology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.ensm.2022.11.045

Cite this

@article{882709163a2947a59ec35d668744da2f,

title = "Implanting single-atom N2-Fe-B2 catalytic sites in carbon hosts to stabilize high-loading and lean-electrolyte lithium-sulfur batteries",

abstract = "Lithium-sulfur (Li-S) batteries suffer from soluble lithium polysulfide (LiPS) shuttling and sluggish redox kinetics. The rational design of carbon-supported single-atom catalysts (SACs) as both LiPS immobilizers and sulfur redox promoters is of great significance for high-loading and lean-electrolyte Li-S batteries. However, the most popular nonpolar porphyrin-like transition metal-nitrogen (M-N4) SACs cannot maximize the catalytic activity of the metal center. Herein, a B, N co-coordinated N2-Fe-B2 SAC embedded in a B, N-rich carbon matrix (denoted as Fe SAs@BCN) is disclosed for the first time to construct state-of-the-art Li-S batteries. We reveal experimentally and theoretically that the asymmetric N2-Fe-B2 configuration not only rapidly captures LiPSs through strong Lewis acid-base interactions, but also greatly catalyzes the bidirectional sulfur redox chemistry by lowering the Li2S deposition/decomposition energy barriers. As such, the well-designed SACs enable Li-S batteries to promise extraordinary durability (82% retention over 1000 cycles at 5 C) and high areal capacities even under harsh sulfur mass loadings. More encouragingly, a 359 Wh kg−1 pouch cell with an ultrahigh loading of 11.6 mg·S cm−2 and a lean electrolyte to sulfur (E/S) ratio of 3 µL mg·S−1 is further demonstrated. This work shows that N2-Fe-B2 SACs hold great promise in realizing high-energy-density Li-S batteries.",

keywords = "Bidirectional sulfur redox, High-energy-density, Lithium-sulfur batteries, N-Fe-B configuration, Single atom catalysts",

author = "Sha Li and Jiande Lin and Bin Chang and Daiwen Yang and Wu, {De Yin} and Junhao Wang and Weijia Zhou and Hong Liu and Shuhui Sun and Li Zhang",

note = "Funding Information: The authors acknowledge financial support from the National Natural Science Foundation of China (NSFC, 21875155 , 22032004 , 51972147 , 52022037 , and 52202366 ), the support of the National Key Research and Development Program of China ( 2021YFA1201502 ), the support of Nanqiang Young Top-notch Talent Fellowship in Xiamen University, Taishan Scholars Project Special Funds ( tsqn201812083 ), and the Natural Sciences and Engineering Research Council of Canada (NSERC). Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2023",

month = jan,

doi = "10.1016/j.ensm.2022.11.045",

language = "English (US)",

volume = "55",

pages = "94--104",

journal = "Energy Storage Materials",

issn = "2405-8297",

publisher = "Elsevier B.V.",

}

TY - JOUR

T1 - Implanting single-atom N2-Fe-B2 catalytic sites in carbon hosts to stabilize high-loading and lean-electrolyte lithium-sulfur batteries

AU - Li, Sha

AU - Lin, Jiande

AU - Chang, Bin

AU - Yang, Daiwen

AU - Wu, De Yin

AU - Wang, Junhao

AU - Zhou, Weijia

AU - Liu, Hong

AU - Sun, Shuhui

AU - Zhang, Li

N1 - Funding Information: The authors acknowledge financial support from the National Natural Science Foundation of China (NSFC, 21875155 , 22032004 , 51972147 , 52022037 , and 52202366 ), the support of the National Key Research and Development Program of China ( 2021YFA1201502 ), the support of Nanqiang Young Top-notch Talent Fellowship in Xiamen University, Taishan Scholars Project Special Funds ( tsqn201812083 ), and the Natural Sciences and Engineering Research Council of Canada (NSERC). Publisher Copyright: © 2022 Elsevier B.V.

PY - 2023/1

Y1 - 2023/1

N2 - Lithium-sulfur (Li-S) batteries suffer from soluble lithium polysulfide (LiPS) shuttling and sluggish redox kinetics. The rational design of carbon-supported single-atom catalysts (SACs) as both LiPS immobilizers and sulfur redox promoters is of great significance for high-loading and lean-electrolyte Li-S batteries. However, the most popular nonpolar porphyrin-like transition metal-nitrogen (M-N4) SACs cannot maximize the catalytic activity of the metal center. Herein, a B, N co-coordinated N2-Fe-B2 SAC embedded in a B, N-rich carbon matrix (denoted as Fe SAs@BCN) is disclosed for the first time to construct state-of-the-art Li-S batteries. We reveal experimentally and theoretically that the asymmetric N2-Fe-B2 configuration not only rapidly captures LiPSs through strong Lewis acid-base interactions, but also greatly catalyzes the bidirectional sulfur redox chemistry by lowering the Li2S deposition/decomposition energy barriers. As such, the well-designed SACs enable Li-S batteries to promise extraordinary durability (82% retention over 1000 cycles at 5 C) and high areal capacities even under harsh sulfur mass loadings. More encouragingly, a 359 Wh kg−1 pouch cell with an ultrahigh loading of 11.6 mg·S cm−2 and a lean electrolyte to sulfur (E/S) ratio of 3 µL mg·S−1 is further demonstrated. This work shows that N2-Fe-B2 SACs hold great promise in realizing high-energy-density Li-S batteries.

AB - Lithium-sulfur (Li-S) batteries suffer from soluble lithium polysulfide (LiPS) shuttling and sluggish redox kinetics. The rational design of carbon-supported single-atom catalysts (SACs) as both LiPS immobilizers and sulfur redox promoters is of great significance for high-loading and lean-electrolyte Li-S batteries. However, the most popular nonpolar porphyrin-like transition metal-nitrogen (M-N4) SACs cannot maximize the catalytic activity of the metal center. Herein, a B, N co-coordinated N2-Fe-B2 SAC embedded in a B, N-rich carbon matrix (denoted as Fe SAs@BCN) is disclosed for the first time to construct state-of-the-art Li-S batteries. We reveal experimentally and theoretically that the asymmetric N2-Fe-B2 configuration not only rapidly captures LiPSs through strong Lewis acid-base interactions, but also greatly catalyzes the bidirectional sulfur redox chemistry by lowering the Li2S deposition/decomposition energy barriers. As such, the well-designed SACs enable Li-S batteries to promise extraordinary durability (82% retention over 1000 cycles at 5 C) and high areal capacities even under harsh sulfur mass loadings. More encouragingly, a 359 Wh kg−1 pouch cell with an ultrahigh loading of 11.6 mg·S cm−2 and a lean electrolyte to sulfur (E/S) ratio of 3 µL mg·S−1 is further demonstrated. This work shows that N2-Fe-B2 SACs hold great promise in realizing high-energy-density Li-S batteries.

KW - Bidirectional sulfur redox

KW - High-energy-density

KW - Lithium-sulfur batteries

KW - N-Fe-B configuration

KW - Single atom catalysts

UR - http://www.scopus.com/inward/record.url?scp=85146244150&partnerID=8YFLogxK

U2 - 10.1016/j.ensm.2022.11.045

DO - 10.1016/j.ensm.2022.11.045

M3 - Article

AN - SCOPUS:85146244150

SN - 2405-8297

VL - 55

SP - 94

EP - 104

JO - Energy Storage Materials

JF - Energy Storage Materials

ER -