A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries
Low electrolyte usage is a key to attaining high-energy-density lithium–sulfur (Li–S) batteries. However, this is still a tremendous challenge for traditional ether-based electrolytes that follow a dissolution–precipitation mechanism. Highly solvating electrolytes, which can facilitate polysulfide d...
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| Format: | Article |
| Language: | English |
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Tsinghua University Press
2024-12-01
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| Series: | Nano Research Energy |
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| Online Access: | https://www.sciopen.com/article/10.26599/NRE.2024.9120126 |
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| author | Zixiong Shi Simil Thomas Zhengnan Tian Dong Guo Zhiming Zhao Yizhou Wang Shuo Li Nimer Wehbe Abdul-Hamid Emwas Osman M. Bakr Omar F. Mohammed Husam N. Alshareef |
| author_facet | Zixiong Shi Simil Thomas Zhengnan Tian Dong Guo Zhiming Zhao Yizhou Wang Shuo Li Nimer Wehbe Abdul-Hamid Emwas Osman M. Bakr Omar F. Mohammed Husam N. Alshareef |
| author_sort | Zixiong Shi |
| collection | DOAJ |
| description | Low electrolyte usage is a key to attaining high-energy-density lithium–sulfur (Li–S) batteries. However, this is still a tremendous challenge for traditional ether-based electrolytes that follow a dissolution–precipitation mechanism. Highly solvating electrolytes, which can facilitate polysulfide dissolution and alter reaction pathway, are considered a promising strategy. Nonetheless, mechanistic understanding and kinetic evaluation remain insufficient while the principle of Li2S nucleation and dissociation has not been elucidated. Herein, we unveil the Li-ion solvation and polysulfide speciation in the solvents with different denticity and donicity. The origin of S3•– radical-directed path and three-dimensional Li2S precipitation in high-donicity electrolytes has been uncovered. It is revealed that ammonium ions enable the facile dissolution and dissociation of Li2S via Lewis acid-base interaction and H···S2– binding. Consequently, Li–S batteries with a low electrolyte and sulfur (E/S) ratio of 5 μL·mgs–1 achieve a high capacity of 1092 mAh·g–1. Even at a harsh E/S ratio of 3 μL·mgs–1 and a high sulfur loading of 4 mg·cm–2, they still sustain a stable operation over 30 cycles. Our work sheds light on the underlying reaction mechanism and rationalizes the design of highly solvating electrolytes, which in turn opens a new avenue for achieving pragmatic lean-electrolyte Li–S batteries. |
| format | Article |
| id | doaj-art-cc7d0209ca0b4d3e82bee8f47a34eee3 |
| institution | Kabale University |
| issn | 2791-0091 2790-8119 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Tsinghua University Press |
| record_format | Article |
| series | Nano Research Energy |
| spelling | doaj-art-cc7d0209ca0b4d3e82bee8f47a34eee32024-12-29T16:10:28ZengTsinghua University PressNano Research Energy2791-00912790-81192024-12-0134e912012610.26599/NRE.2024.9120126A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteriesZixiong Shi0Simil Thomas1Zhengnan Tian2Dong Guo3Zhiming Zhao4Yizhou Wang5Shuo Li6Nimer Wehbe7Abdul-Hamid Emwas8Osman M. Bakr9Omar F. Mohammed10Husam N. Alshareef11Materials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaAdvanced Membranes and Porous Materials Center (AMPMC), King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaCore Labs, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaCore Labs, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaAdvanced Membranes and Porous Materials Center (AMPMC), King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaMaterials Science and Engineering, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaLow electrolyte usage is a key to attaining high-energy-density lithium–sulfur (Li–S) batteries. However, this is still a tremendous challenge for traditional ether-based electrolytes that follow a dissolution–precipitation mechanism. Highly solvating electrolytes, which can facilitate polysulfide dissolution and alter reaction pathway, are considered a promising strategy. Nonetheless, mechanistic understanding and kinetic evaluation remain insufficient while the principle of Li2S nucleation and dissociation has not been elucidated. Herein, we unveil the Li-ion solvation and polysulfide speciation in the solvents with different denticity and donicity. The origin of S3•– radical-directed path and three-dimensional Li2S precipitation in high-donicity electrolytes has been uncovered. It is revealed that ammonium ions enable the facile dissolution and dissociation of Li2S via Lewis acid-base interaction and H···S2– binding. Consequently, Li–S batteries with a low electrolyte and sulfur (E/S) ratio of 5 μL·mgs–1 achieve a high capacity of 1092 mAh·g–1. Even at a harsh E/S ratio of 3 μL·mgs–1 and a high sulfur loading of 4 mg·cm–2, they still sustain a stable operation over 30 cycles. Our work sheds light on the underlying reaction mechanism and rationalizes the design of highly solvating electrolytes, which in turn opens a new avenue for achieving pragmatic lean-electrolyte Li–S batteries.https://www.sciopen.com/article/10.26599/NRE.2024.9120126donicitys3•– radicalli2s dissociationlean-electrolyteli–s batteries |
| spellingShingle | Zixiong Shi Simil Thomas Zhengnan Tian Dong Guo Zhiming Zhao Yizhou Wang Shuo Li Nimer Wehbe Abdul-Hamid Emwas Osman M. Bakr Omar F. Mohammed Husam N. Alshareef A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries Nano Research Energy donicity s3•– radical li2s dissociation lean-electrolyte li–s batteries |
| title | A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries |
| title_full | A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries |
| title_fullStr | A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries |
| title_full_unstemmed | A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries |
| title_short | A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries |
| title_sort | tailored highly solvating electrolyte toward ultra lean electrolyte li s batteries |
| topic | donicity s3•– radical li2s dissociation lean-electrolyte li–s batteries |
| url | https://www.sciopen.com/article/10.26599/NRE.2024.9120126 |
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