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学者姓名：雷杰
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Abstract ：
Wide operation temperature is the crucial objective for an energy storage system that can be applied under harsh environmental conditions. For lithium-sulfur batteries, the “shuttle effect” of polysulfide intermediates will aggravate with the temperature increasing, while the reaction kinetics decreases sharply as the temperature decreasing. In particular, sulfur reaction mechanism at low temperatures seems to be quite different from that at room temperature. Here, through in situ Raman and electrochemical impedance spectroscopy studies, the newly emerged platform at cryogenic temperature corresponds to the reduction process of Li2S8 to Li2S4, which will be another rate-determining step of sulfur conversion reaction, in addition to the solid-phase conversion process of Li2S4 to Li2S2/Li2S at low temperatures. Porous bismuth vanadate (BiVO4) spheres are designed as sulfur host material, which achieve the rapid snap-transfer-catalytic process by shortening lithium-ion transport pathway and accelerating the targeted rate-determining steps. Such promoting effect greatly inhibits severe “shuttle effect” at high temperatures and simultaneously improves sulfur conversion efficiency in the cryogenic environment. The cell with the porous BiVO4 spheres as the host exhibits excellent rate capability and cycle performance under wide working temperatures. © 2024 Wiley-VCH GmbH.
Keyword ：
bismuth vanadate bismuth vanadate lithium-sulfur batteries lithium-sulfur batteries rate-determinate step rate-determinate step reaction mechanism reaction mechanism wide temperature range wide temperature range
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| GB/T 7714 | Deng, D.-R. , Xiong, H.-J. , Luo, Y.-L. et al. Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range [J]. | Advanced Materials , 2024 , 36 (39) . |
| MLA | Deng, D.-R. et al. "Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range" . | Advanced Materials 36 . 39 (2024) . |
| APA | Deng, D.-R. , Xiong, H.-J. , Luo, Y.-L. , Yu, K.-M. , Weng, J.-C. , Li, G.-F. et al. Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range . | Advanced Materials , 2024 , 36 (39) . |
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Abstract ：
The development of electrocatalysts with high catalytic activity is conducive to enhancing polysulfides adsorption and reducing activation energy of polysulfides conversion, which can effectively reduce polysulfide shuttling in Li-S batteries. Herein, a novel catalyst NiCo-MoOx/rGO (rGO = reduced graphene oxides) with ultra-nanometer scale and high dispersity is derived from the Anderson-type polyoxometalate precursors, which are electrostatically assembled on the multilayer rGO. The catalyst material possesses dual active sites, in which Ni-doped MoOx exhibits strong polysulfide anchoring ability, while Co-doped MoOx facilitates the polysulfides conversion reaction kinetics, thus breaking the Sabatier effect in the conventional electrocatalytic process. In addition, the prepared NiCo-MoOx/rGO modified PP separator (NiCo-MoOx/rGO@PP) can serve as a physical barrier to further inhibit the polysulfide shuttling effect and realize the rapid Li+ migration. The results demonstrate that Li-S coin cell with NiCo-MoOx/rGO@PP separator shows excellent cycling performance with the discharge capacity of 680 mAh·g−1 after 600 cycles at 1 C and the capacity fading of 0.064% per cycle. The rate performance is also impressive with the remained capacity of 640 mAh·g−1 after 200 cycles even at 4 C. When the sulfur loading is 4.0 mg·cm−2 and electrolyte volume/sulfur mass ratio (E/S) ratio is 6.0 μL·mg−1, a specific capacity of 830 mAh·g−1 is achieved after 200 cycles with a capacity decay of 0.049% per cycle. More importantly, the cell with NiCo-MoOx/rGO@PP separator exhibits cycling performance under wide operating temperature with the reversible capacities of 518, 715, and 915 mAh·g−1 after 100 cycles at −20, 0, and 60 °C, respectively. This study provides a new design approach of highly efficient catalysts for sulfur conversion reaction in Li-S batteries. (Figure presented.) © Tsinghua University Press 2024.
Keyword ：
adsorption and catalysis dual-sites adsorption and catalysis dual-sites doped molybdenum oxide doped molybdenum oxide lithium-sulfur batteries lithium-sulfur batteries separator modification separator modification wide temperature wide temperature
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| GB/T 7714 | Chen, J. , Lei, J. , Zhou, J. et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature [J]. | Nano Research , 2024 , 17 (11) : 9651-9661 . |
| MLA | Chen, J. et al. "Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature" . | Nano Research 17 . 11 (2024) : 9651-9661 . |
| APA | Chen, J. , Lei, J. , Zhou, J. , Chen, X. , Deng, R. , Qian, M. et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature . | Nano Research , 2024 , 17 (11) , 9651-9661 . |
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Abstract ：
Wide operation temperature is the crucial objective for an energy storage system that can be applied under harsh environmental conditions. For lithium-sulfur batteries, the "shuttle effect" of polysulfide intermediates will aggravate with the temperature increasing, while the reaction kinetics decreases sharply as the temperature decreasing. In particular, sulfur reaction mechanism at low temperatures seems to be quite different from that at room temperature. Here, through in situ Raman and electrochemical impedance spectroscopy studies, the newly emerged platform at cryogenic temperature corresponds to the reduction process of Li2S8 to Li2S4, which will be another rate-determining step of sulfur conversion reaction, in addition to the solid-phase conversion process of Li2S4 to Li2S2/Li2S at low temperatures. Porous bismuth vanadate (BiVO4) spheres are designed as sulfur host material, which achieve the rapid snap-transfer-catalytic process by shortening lithium-ion transport pathway and accelerating the targeted rate-determining steps. Such promoting effect greatly inhibits severe "shuttle effect" at high temperatures and simultaneously improves sulfur conversion efficiency in the cryogenic environment. The cell with the porous BiVO4 spheres as the host exhibits excellent rate capability and cycle performance under wide working temperatures.
Keyword ：
bismuth vanadate bismuth vanadate lithium-sulfur batteries lithium-sulfur batteries rate-determinate step rate-determinate step reaction mechanism reaction mechanism wide temperature range wide temperature range
Cite：
Copy from the list or Export to your reference management。
| GB/T 7714 | Deng, Ding-Rong , Xiong, Hai-Ji , Luo, Yu-Lin et al. Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range [J]. | ADVANCED MATERIALS , 2024 , 36 (39) . |
| MLA | Deng, Ding-Rong et al. "Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range" . | ADVANCED MATERIALS 36 . 39 (2024) . |
| APA | Deng, Ding-Rong , Xiong, Hai-Ji , Luo, Yu-Lin , Yu, Kai-Min , Weng, Jian-Chun , Li, Gui-Fang et al. Accelerating the Rate-Determining Steps of Sulfur Conversion Reaction for Lithium-Sulfur Batteries Working at an Ultrawide Temperature Range . | ADVANCED MATERIALS , 2024 , 36 (39) . |
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Abstract ：
The development of electrocatalysts with high catalytic activity is conducive to enhancing polysulfides adsorption and reducing activation energy of polysulfides conversion, which can effectively reduce polysulfide shuttling in Li-S batteries. Herein, a novel catalyst NiCo-MoOx/rGO (rGO = reduced graphene oxides) with ultra-nanometer scale and high dispersity is derived from the Anderson-type polyoxometalate precursors, which are electrostatically assembled on the multilayer rGO. The catalyst material possesses dual active sites, in which Ni-doped MoOx exhibits strong polysulfide anchoring ability, while Co-doped MoOx facilitates the polysulfides conversion reaction kinetics, thus breaking the Sabatier effect in the conventional electrocatalytic process. In addition, the prepared NiCo-MoOx/rGO modified PP separator (NiCo-MoOx/rGO@PP) can serve as a physical barrier to further inhibit the polysulfide shuttling effect and realize the rapid Li+ migration. The results demonstrate that Li-S coin cell with NiCo-MoOx/rGO@PP separator shows excellent cycling performance with the discharge capacity of 680 mAhg-1 after 600 cycles at 1 C and the capacity fading of 0.064% per cycle. The rate performance is also impressive with the remained capacity of 640 mAhg-1 after 200 cycles even at 4 C. When the sulfur loading is 4.0 mgcm-2 and electrolyte volume/sulfur mass ratio (E/S) ratio is 6.0 mu Lmg-1, a specific capacity of 830 mAhg-1 is achieved after 200 cycles with a capacity decay of 0.049% per cycle. More importantly, the cell with NiCo-MoOx/rGO@PP separator exhibits cycling performance under wide operating temperature with the reversible capacities of 518, 715, and 915 mAhg-1 after 100 cycles at -20, 0, and 60 degrees C, respectively. This study provides a new design approach of highly efficient catalysts for sulfur conversion reaction in Li-S batteries.
Keyword ：
adsorption and catalysis dual-sites adsorption and catalysis dual-sites doped molybdenum oxide doped molybdenum oxide lithium-sulfur batteries lithium-sulfur batteries separator modification separator modification wide temperature wide temperature
Cite：
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| GB/T 7714 | Chen, Jieshuangyang , Lei, Jie , Zhou, Jinwei et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature [J]. | NANO RESEARCH , 2024 , 17 (11) : 9651-9661 . |
| MLA | Chen, Jieshuangyang et al. "Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature" . | NANO RESEARCH 17 . 11 (2024) : 9651-9661 . |
| APA | Chen, Jieshuangyang , Lei, Jie , Zhou, Jinwei , Chen, Xuanfeng , Deng, Rongyu , Qian, Mingzhi et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature . | NANO RESEARCH , 2024 , 17 (11) , 9651-9661 . |
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Abstract ：
Alloy catalyst is considered to be an important strategy to solve the shuttle effect and sluggish kinetics of lithium-sulfur batteries (LSBs). However, the effect of the electronic structure of the alloy catalyst on the sulfur conversion process has not been effectively analyzed. In this paper, based on alloying strategy, the electronic structure of such a FeCoNi catalyst is regulated and optimized, and the sulfur adsorption configuration and catalytic conversion process are defined. The in situ Raman spectroscopy and the density functional theory (DFT) are employed to deeply understand the catalytic mechanism of such a sulfur conversion. A cell with FeCoNi modified separator delivers an ultra-low capacity attenuation of 0.056% per cycle over 1000 cycles at 3 C. The outstanding anti-self-discharge performance of 8.1% over 7 days is also achieved. Furthermore, the obtained cell with a high sulfur loading of 9.7 mg cm-2 and lean electrolyte of 5.6 mu L mgs-1 exhibits 81% capacity retention after 100 cycles, providing a research prospect for the practical application of lithium-sulfur batteries. Based on the intrinsic electronic structure of the alloy catalyst, the surface electronic reconstruction process of the alloy catalyst is analyzed, and its catalytic mechanism in the sulfur conversion process is elucidated, which provides a new idea for the development of alloy catalyst and lithium sulfur battery. image
Keyword ：
chemisorption chemisorption electrocatalyst electrocatalyst electrochemical kinetics electrochemical kinetics FeCoNi FeCoNi lithium-sulfur batteries lithium-sulfur batteries
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| GB/T 7714 | Zuo, Yinze , Jiao, Xuechao , Huang, Zheng et al. Surface Electron Reconstruction of Catalyst Through Alloying Strategy for Accelerating Sulfur Conversion in Lithium-Sulfur Batteries [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (44) . |
| MLA | Zuo, Yinze et al. "Surface Electron Reconstruction of Catalyst Through Alloying Strategy for Accelerating Sulfur Conversion in Lithium-Sulfur Batteries" . | ADVANCED FUNCTIONAL MATERIALS 34 . 44 (2024) . |
| APA | Zuo, Yinze , Jiao, Xuechao , Huang, Zheng , Lei, Jie , Liu, Mingquan , Dong, Li et al. Surface Electron Reconstruction of Catalyst Through Alloying Strategy for Accelerating Sulfur Conversion in Lithium-Sulfur Batteries . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (44) . |
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