Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction
Abstract The sluggish kinetics in multistep sulfur redox reaction with different energy requirements for each step, is considered as the crucial handicap of lithium–sulfur (Li–S) batteries. Designing an electron reservoir, which can dynamically release electron to/accept electron from sulfur species...
| Main Authors: | , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Wiley
2023-01-01
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| Series: | InfoMat |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/inf2.12381 |
| _version_ | 1828049538504458240 |
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| author | Shuang Yu Shuo Yang Dong Cai Huagui Nie Xuemei Zhou Tingting Li Ce Liang Haohao Wang Yangyang Dong Rui Xu Guoyong Fang Jinjie Qian Yongjie Ge Yue Hu Zhi Yang |
| author_facet | Shuang Yu Shuo Yang Dong Cai Huagui Nie Xuemei Zhou Tingting Li Ce Liang Haohao Wang Yangyang Dong Rui Xu Guoyong Fang Jinjie Qian Yongjie Ge Yue Hu Zhi Yang |
| author_sort | Shuang Yu |
| collection | DOAJ |
| description | Abstract The sluggish kinetics in multistep sulfur redox reaction with different energy requirements for each step, is considered as the crucial handicap of lithium–sulfur (Li–S) batteries. Designing an electron reservoir, which can dynamically release electron to/accept electron from sulfur species during discharge/charge, is the ideal strategy for realizing stepwise and dual‐directional polysulfide electrocatalysis. Herein, a single Tb3+/4+ oxide with moderate unfilled f orbital is synthetized as an electron reservoir to optimize polysulfide adsorption via Tb–S and N···Li bonds, reduce activation energy barrier, expedite electron/Li+ transport, and selectively catalyze both long‐chain and short‐chain polysulfide conversions during charge and discharge. As a result, Tb electron reservoir enables stable operation of low‐capacity decay (0.087% over 500 cycles at 1 C), high sulfur loading (5.2 mg cm−2) and electrolyte‐starved (7.5 μL mg−1) Li–S batteries. This work could unlock the potential of f orbital engineering for high‐energy battery systems. |
| first_indexed | 2024-04-10T19:11:28Z |
| format | Article |
| id | doaj.art-baa83b3695ba4d89a524cfba1f923493 |
| institution | Directory Open Access Journal |
| issn | 2567-3165 |
| language | English |
| last_indexed | 2024-04-10T19:11:28Z |
| publishDate | 2023-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | InfoMat |
| spelling | doaj.art-baa83b3695ba4d89a524cfba1f9234932023-01-30T13:26:47ZengWileyInfoMat2567-31652023-01-0151n/an/a10.1002/inf2.12381Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reactionShuang Yu0Shuo Yang1Dong Cai2Huagui Nie3Xuemei Zhou4Tingting Li5Ce Liang6Haohao Wang7Yangyang Dong8Rui Xu9Guoyong Fang10Jinjie Qian11Yongjie Ge12Yue Hu13Zhi Yang14Key Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaCollege of Electrical and Electronic Engineering Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou People's Republic of ChinaAbstract The sluggish kinetics in multistep sulfur redox reaction with different energy requirements for each step, is considered as the crucial handicap of lithium–sulfur (Li–S) batteries. Designing an electron reservoir, which can dynamically release electron to/accept electron from sulfur species during discharge/charge, is the ideal strategy for realizing stepwise and dual‐directional polysulfide electrocatalysis. Herein, a single Tb3+/4+ oxide with moderate unfilled f orbital is synthetized as an electron reservoir to optimize polysulfide adsorption via Tb–S and N···Li bonds, reduce activation energy barrier, expedite electron/Li+ transport, and selectively catalyze both long‐chain and short‐chain polysulfide conversions during charge and discharge. As a result, Tb electron reservoir enables stable operation of low‐capacity decay (0.087% over 500 cycles at 1 C), high sulfur loading (5.2 mg cm−2) and electrolyte‐starved (7.5 μL mg−1) Li–S batteries. This work could unlock the potential of f orbital engineering for high‐energy battery systems.https://doi.org/10.1002/inf2.12381electronic reservoirlithium–sulfur batterysulfur redox reaction kineticsunfilled f orbital |
| spellingShingle | Shuang Yu Shuo Yang Dong Cai Huagui Nie Xuemei Zhou Tingting Li Ce Liang Haohao Wang Yangyang Dong Rui Xu Guoyong Fang Jinjie Qian Yongjie Ge Yue Hu Zhi Yang Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction InfoMat electronic reservoir lithium–sulfur battery sulfur redox reaction kinetics unfilled f orbital |
| title | Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction |
| title_full | Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction |
| title_fullStr | Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction |
| title_full_unstemmed | Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction |
| title_short | Regulating f orbital of Tb electronic reservoir to activate stepwise and dual‐directional sulfur conversion reaction |
| title_sort | regulating f orbital of tb electronic reservoir to activate stepwise and dual directional sulfur conversion reaction |
| topic | electronic reservoir lithium–sulfur battery sulfur redox reaction kinetics unfilled f orbital |
| url | https://doi.org/10.1002/inf2.12381 |
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