Surface-localized phase mediation accelerates quasi-solid-state reaction kinetics in sulfur batteries

被引:10
作者
Liu, Yatao [1 ,2 ]
An, Yun [1 ]
Fang, Chi [3 ]
Ye, Yaokun [3 ]
An, Yifeng [1 ]
He, Mengxue [1 ]
Jia, Yongfeng [1 ]
Hong, Xufeng [1 ]
Liu, Yumei [1 ]
Gao, Song [1 ]
Hao, Yizhou [4 ]
Chen, Jianhao [4 ]
Zheng, Jiaxin [3 ]
Lu, Yunfeng [2 ,5 ]
Zou, Ruqiang [1 ]
Pang, Quanquan [1 ]
机构
[1] Peking Univ, Sch Mat Sci & Engn, Beijing Key Lab Theory & Technol Adv Battery Mat, Beijing, Peoples R China
[2] Beijing Univ Chem Technol, Coll Chem Engn, State Key Lab Organ Inorgan Composites, Beijing, Peoples R China
[3] Peking Univ, Sch Adv Mat, Shenzhen Grad Sch, Shenzhen, Peoples R China
[4] Peking Univ, Int Ctr Quantum Mat, Sch Phys, Beijing, Peoples R China
[5] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金; 北京市自然科学基金; 国家重点研发计划;
关键词
LI-S BATTERIES; ENERGY DENSITY; LITHIUM; ELECTROLYTES; SOLVENT; CATHODES;
D O I
10.1038/s41557-025-01735-w
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Lithium-sulfur batteries promise high energy density storage but show poor stabilities owing to uncontrolled polysulfide dissolution. Although limiting polysulfide solvation to establish quasi-solid-state sulfur reaction can decouple electrode reactions from the electrolyte volume, this approach suffers from slow reaction kinetics. Here we propose a surface-localized polysulfide-solvation strategy to mediate the reaction of 'quasi-solid' polysulfide by leveraging an organic phase mediator with a weakly solvating electrolyte. This electrolyte restricts polysulfide dissolution globally while the phase mediator complexes with the surface polysulfide, promoting polysulfide solvation at the surface and facilitating fast surface-localized solution-phase sulfur reactions. Lithium-sulfur batteries using surface-localized phase mediation show excellent rate performance with 494 mA h g-1-sulfur at 16 C and stabilized cycling for 300 cycles with 90.2% capacity retention. The strategy enables steady operation of a 2.4 Ah 331 Wh kg-1 pouch cell. Our work highlights the advantages of surface phase mediation in controlling electrode reaction pathways and kinetics via electrolyte rational design.
引用
收藏
页码:614 / 623
页数:13
相关论文
共 56 条
[1]   Why charging Li-air batteries with current low-voltage mediators is slow and singlet oxygen does not explain degradation [J].
Ahn, Sunyhik ;
Zor, Ceren ;
Yang, Sixie ;
Lagnoni, Marco ;
Dewar, Daniel ;
Nimmo, Tammy ;
Chau, Chloe ;
Jenkins, Max ;
Kibler, Alexander J. ;
Pateman, Alexander ;
Rees, Gregory J. ;
Gao, Xiangwen ;
Adamson, Paul ;
Grobert, Nicole ;
Bertei, Antonio ;
Johnson, Lee R. ;
Bruce, Peter G. .
NATURE CHEMISTRY, 2023, 15 (07) :1022-+
[2]   SEI growth on Lithium metal anodes in solid-state batteries quantified with coulometric titration time analysis [J].
Aktekin, Burak ;
Riegger, Luise M. ;
Otto, Svenja-K. ;
Fuchs, Till ;
Henss, Anja ;
Janek, Juergen .
NATURE COMMUNICATIONS, 2023, 14 (01)
[3]   Regulating the Hidden Solvation-Ion-Exchange in Concentrated Electrolytes for Stable and Safe Lithium Metal Batteries [J].
Amine, Rachid ;
Liu, Jianzhao ;
Acznik, Ilona ;
Sheng, Tian ;
Lota, Katarzyna ;
Sun, Hui ;
Sun, Cheng-Jun ;
Fic, Krzysztof ;
Zuo, Xiaobing ;
Ren, Yang ;
Abd El-Hady, Deia ;
Alshitari, Wael ;
Al-Bogami, Abdullah S. ;
Chen, Zonghai ;
Amine, Khalil ;
Xu, Gui-Liang .
ADVANCED ENERGY MATERIALS, 2020, 10 (25)
[4]   Triarylmethyl cation redox mediators enhance Li-O2 battery discharge capacities [J].
Askins, Erik J. ;
Zoric, Marija R. ;
Li, Matthew ;
Amine, Rachid ;
Amine, Khalil ;
Curtiss, Larry A. ;
Glusac, Ksenija D. .
NATURE CHEMISTRY, 2023, 15 (09) :1247-+
[5]   Energy demand reduction options for meeting national zero-emission targets in the United Kingdom [J].
Barrett, John ;
Pye, Steve ;
Betts-Davies, Sam ;
Broad, Oliver ;
Price, James ;
Eyre, Nick ;
Anable, Jillian ;
Brand, Christian ;
Bennett, George ;
Carr-Whitworth, Rachel ;
Garvey, Alice ;
Giesekam, Jannik ;
Marsden, Greg ;
Norman, Jonathan ;
Oreszczyn, Tadj ;
Ruyssevelt, Paul ;
Scott, Kate .
NATURE ENERGY, 2022, 7 (08) :726-735
[6]   The unique chemistry of thiuram polysulfides enables energy dense lithium batteries [J].
Bhargav, Amruth ;
Ma, Ying ;
Shashikala, Kollur ;
Cui, Yi ;
Losovyj, Yaroslav ;
Fu, Yongzhu .
JOURNAL OF MATERIALS CHEMISTRY A, 2017, 5 (47) :25005-25013
[7]   Platinum Nanocrystals Embedded in Three-Dimensional Graphene for High-Performance Li-O2 Batteries [J].
Cao, Dong ;
Hao, Yizhou ;
Wang, Yahui ;
Bai, Ying ;
Li, Yu ;
Wang, Xinran ;
Chen, Jianhao ;
Wu, Chuan .
ACS APPLIED MATERIALS & INTERFACES, 2022, 14 (36) :40921-40929
[8]   Monolithic solid-electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization [J].
Cao, Xia ;
Ren, Xiaodi ;
Zou, Lianfeng ;
Engelhard, Mark H. ;
Huang, William ;
Wang, Hansen ;
Matthews, Bethany E. ;
Lee, Hongkyung ;
Niu, Chaojiang ;
Arey, Bruce W. ;
Cui, Yi ;
Wang, Chongmin ;
Xiao, Jie ;
Liu, Jun ;
Xu, Wu ;
Zhang, Ji-Guang .
NATURE ENERGY, 2019, 4 (09) :796-805
[9]   Coordination of Lithium Ion with Ethylene Carbonate Electrolyte Solvent: A Computational Study [J].
Ding, Wenhui ;
Lei, Xueling ;
Ouyang, Chuying .
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, 2016, 116 (02) :97-102
[10]   Electrodeposition Kinetics in Li-S Batteries: Effects of Low Electrolyte/Sulfur Ratios and Deposition Surface Composition [J].
Fan, Frank Y. ;
Chiang, Yet-Ming .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2017, 164 (04) :A917-A922