Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries
The shuttling effect of soluble lithium polysulfides (LiPSs) and the sluggish conversion kinetics of polysulfides into insoluble Li<sub>2</sub>S<sub>2</sub>/Li<sub>2</sub>S severely hinders the practical application of Li-S batteries. Advanced catalysts can captur...
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MDPI AG
2022-10-01
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| Series: | Nanomaterials |
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| Online Access: | https://www.mdpi.com/2079-4991/12/20/3551 |
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| author | Chong Wang Jian-Hao Lu An-Bang Wang Hao Zhang Wei-Kun Wang Zhao-Qing Jin Li-Zhen Fan |
| author_facet | Chong Wang Jian-Hao Lu An-Bang Wang Hao Zhang Wei-Kun Wang Zhao-Qing Jin Li-Zhen Fan |
| author_sort | Chong Wang |
| collection | DOAJ |
| description | The shuttling effect of soluble lithium polysulfides (LiPSs) and the sluggish conversion kinetics of polysulfides into insoluble Li<sub>2</sub>S<sub>2</sub>/Li<sub>2</sub>S severely hinders the practical application of Li-S batteries. Advanced catalysts can capture and accelerate the liquid–solid conversion of polysulfides. Herein, we try to make use of bismuth tantalum oxide with oxygen vacancies as an electrocatalyst to catalyze the conversion of LiPSs by reducing the sulfur reduction reaction (SRR) nucleation energy barrier. Oxygen vacancies in Bi<sub>4</sub>TaO<sub>7</sub> nanoparticles alter the electron band structure to improve instinct electronic conductivity and catalytic activity. In addition, the defective surface could provide unsaturated bonds around the vacancies to enhance the chemisorption capability with LiPSs. Hence, a multidimensional carbon (super P/CNT/Graphene) standing sulfur cathode is prepared by coating oxygen vacancies Bi<sub>4</sub>TaO<sub>7−x</sub> nanoparticles, in which the multidimensional carbon (MC) with micropores structure can host sulfur and provide a fast electron/ion pathway, while the outer-coated oxygen vacancies with Bi<sub>4</sub>TaO<sub>7−x</sub> with improved electronic conductivity and strong affinities for polysulfides can work as an adsorptive and conductive protective layer to achieve the physical restriction and chemical immobilization of lithium polysulfides as well as speed up their catalytic conversion. Benefiting from the synergistic effects of different components, the S/C@Bi<sub>3</sub>TaO<sub>7−x</sub> coin cell cathode shows superior cycling and rate performance. Even under a high level of sulfur loading of 9.6 mg cm<sup>−2</sup>, a relatively high initial areal capacity of 10.20 mAh cm<sup>−2</sup> and a specific energy density of 300 Wh kg<sup>−1</sup> are achieved with a low electrolyte/sulfur ratio of 3.3 µL mg<sup>−1</sup>. Combined with experimental results and theoretical calculations, the mechanism by which the Bi<sub>4</sub>TaO<sub>7</sub> with oxygen vacancies promotes the kinetics of polysulfide conversion reactions has been revealed. The design of the multiple confined cathode structure provides physical and chemical adsorption, fast charge transfer, and catalytic conversion for polysulfides. |
| first_indexed | 2024-03-09T19:40:02Z |
| format | Article |
| id | doaj.art-00446d1b20684eca810d4a60bce54673 |
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| language | English |
| last_indexed | 2024-03-09T19:40:02Z |
| publishDate | 2022-10-01 |
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| series | Nanomaterials |
| spelling | doaj.art-00446d1b20684eca810d4a60bce546732023-11-24T01:39:01ZengMDPI AGNanomaterials2079-49912022-10-011220355110.3390/nano12203551Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur BatteriesChong Wang0Jian-Hao Lu1An-Bang Wang2Hao Zhang3Wei-Kun Wang4Zhao-Qing Jin5Li-Zhen Fan6Beijing Advanced Innovation Center for Materials Genome Engineering, Institute of Advanced Materials and Technology, University of Science and Technology Beijing, Beijing 100083, ChinaMilitary Power Sources Research and Development Center, Research Institute of Chemical Defense, Beijing 100191, ChinaMilitary Power Sources Research and Development Center, Research Institute of Chemical Defense, Beijing 100191, ChinaMilitary Power Sources Research and Development Center, Research Institute of Chemical Defense, Beijing 100191, ChinaMilitary Power Sources Research and Development Center, Research Institute of Chemical Defense, Beijing 100191, ChinaMilitary Power Sources Research and Development Center, Research Institute of Chemical Defense, Beijing 100191, ChinaBeijing Advanced Innovation Center for Materials Genome Engineering, Institute of Advanced Materials and Technology, University of Science and Technology Beijing, Beijing 100083, ChinaThe shuttling effect of soluble lithium polysulfides (LiPSs) and the sluggish conversion kinetics of polysulfides into insoluble Li<sub>2</sub>S<sub>2</sub>/Li<sub>2</sub>S severely hinders the practical application of Li-S batteries. Advanced catalysts can capture and accelerate the liquid–solid conversion of polysulfides. Herein, we try to make use of bismuth tantalum oxide with oxygen vacancies as an electrocatalyst to catalyze the conversion of LiPSs by reducing the sulfur reduction reaction (SRR) nucleation energy barrier. Oxygen vacancies in Bi<sub>4</sub>TaO<sub>7</sub> nanoparticles alter the electron band structure to improve instinct electronic conductivity and catalytic activity. In addition, the defective surface could provide unsaturated bonds around the vacancies to enhance the chemisorption capability with LiPSs. Hence, a multidimensional carbon (super P/CNT/Graphene) standing sulfur cathode is prepared by coating oxygen vacancies Bi<sub>4</sub>TaO<sub>7−x</sub> nanoparticles, in which the multidimensional carbon (MC) with micropores structure can host sulfur and provide a fast electron/ion pathway, while the outer-coated oxygen vacancies with Bi<sub>4</sub>TaO<sub>7−x</sub> with improved electronic conductivity and strong affinities for polysulfides can work as an adsorptive and conductive protective layer to achieve the physical restriction and chemical immobilization of lithium polysulfides as well as speed up their catalytic conversion. Benefiting from the synergistic effects of different components, the S/C@Bi<sub>3</sub>TaO<sub>7−x</sub> coin cell cathode shows superior cycling and rate performance. Even under a high level of sulfur loading of 9.6 mg cm<sup>−2</sup>, a relatively high initial areal capacity of 10.20 mAh cm<sup>−2</sup> and a specific energy density of 300 Wh kg<sup>−1</sup> are achieved with a low electrolyte/sulfur ratio of 3.3 µL mg<sup>−1</sup>. Combined with experimental results and theoretical calculations, the mechanism by which the Bi<sub>4</sub>TaO<sub>7</sub> with oxygen vacancies promotes the kinetics of polysulfide conversion reactions has been revealed. The design of the multiple confined cathode structure provides physical and chemical adsorption, fast charge transfer, and catalytic conversion for polysulfides.https://www.mdpi.com/2079-4991/12/20/3551lithium–sulfur batteryoxygen vacancieselectrochemical performancehigh areal mass loading |
| spellingShingle | Chong Wang Jian-Hao Lu An-Bang Wang Hao Zhang Wei-Kun Wang Zhao-Qing Jin Li-Zhen Fan Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries Nanomaterials lithium–sulfur battery oxygen vacancies electrochemical performance high areal mass loading |
| title | Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries |
| title_full | Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries |
| title_fullStr | Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries |
| title_full_unstemmed | Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries |
| title_short | Oxygen Vacancies in Bismuth Tantalum Oxide to Anchor Polysulfide and Accelerate the Sulfur Evolution Reaction in Lithium–Sulfur Batteries |
| title_sort | oxygen vacancies in bismuth tantalum oxide to anchor polysulfide and accelerate the sulfur evolution reaction in lithium sulfur batteries |
| topic | lithium–sulfur battery oxygen vacancies electrochemical performance high areal mass loading |
| url | https://www.mdpi.com/2079-4991/12/20/3551 |
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