Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries
Abstract Lithium–sulfur batteries (LSBs) have emerged as promising power sources for high‐performance devices such as electric vehicles. However, the poor energy density of LSBs owing to polysulfide shuttling and passivation has limited their further market penetration. To mitigate this challenge, t...
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2021
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oai:doaj.org-article:73d9dccf92034b0aa0efea3838398d072021-11-24T14:45:31ZElectrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries2637-936810.1002/cey2.152https://doaj.org/article/73d9dccf92034b0aa0efea3838398d072021-11-01T00:00:00Zhttps://doi.org/10.1002/cey2.152https://doaj.org/toc/2637-9368Abstract Lithium–sulfur batteries (LSBs) have emerged as promising power sources for high‐performance devices such as electric vehicles. However, the poor energy density of LSBs owing to polysulfide shuttling and passivation has limited their further market penetration. To mitigate this challenge, two‐dimensional (2D) siloxene (2DSi), a Si‐based analog of graphene, is utilized as an additive for sulfur cathodes. The 2DSi is fabricated on a large scale by simple solvent extraction of calcium disilicide to form a thin‐layered structure of Si planes functionalized with vertically aligned hydroxyl groups in the 2DSi. The stoichiometric reaction of 2DSi with polysulfides generates a thiosulfate redox mediator, secures the intercalation pathway, and reveals Lewis acidic sites within the siloxene galleries. The 2DSi utilizes the corresponding in‐situ‐formed electrocatalyst, the 2D confinement effect of the layered structure, and the surface affinity based on Lewis acid–base interaction to improve the energy density of 2DSi‐based LSB cells. Combined with the commercial carbon‐based current collector, 2DSi‐based LSB cells achieve a volumetric energy density of 612 Wh Lcell−1 at 1 mA cm−2 with minor degradation of 0.17% per cycle, which rivals those of state‐of‐the‐art LSBs. This study presents a method for the industrial production of high‐energy‐dense LSBs.Hui‐Ju KangJae‐Woo ParkHyun Jin HwangHeejin KimKwang‐Suk JangXiulei JiHae Jin KimWon Bin ImYoung‐Si JunWileyarticle2D confinement effectsLewis acid–base interactionslithium–sulfur batteriessiloxenesthiosulfate–polythionate redox coupleProduction of electric energy or power. Powerplants. Central stationsTK1001-1841ENCarbon Energy, Vol 3, Iss 6, Pp 976-990 (2021) |
| institution |
DOAJ |
| collection |
DOAJ |
| language |
EN |
| topic |
2D confinement effects Lewis acid–base interactions lithium–sulfur batteries siloxenes thiosulfate–polythionate redox couple Production of electric energy or power. Powerplants. Central stations TK1001-1841 |
| spellingShingle |
2D confinement effects Lewis acid–base interactions lithium–sulfur batteries siloxenes thiosulfate–polythionate redox couple Production of electric energy or power. Powerplants. Central stations TK1001-1841 Hui‐Ju Kang Jae‐Woo Park Hyun Jin Hwang Heejin Kim Kwang‐Suk Jang Xiulei Ji Hae Jin Kim Won Bin Im Young‐Si Jun Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| description |
Abstract Lithium–sulfur batteries (LSBs) have emerged as promising power sources for high‐performance devices such as electric vehicles. However, the poor energy density of LSBs owing to polysulfide shuttling and passivation has limited their further market penetration. To mitigate this challenge, two‐dimensional (2D) siloxene (2DSi), a Si‐based analog of graphene, is utilized as an additive for sulfur cathodes. The 2DSi is fabricated on a large scale by simple solvent extraction of calcium disilicide to form a thin‐layered structure of Si planes functionalized with vertically aligned hydroxyl groups in the 2DSi. The stoichiometric reaction of 2DSi with polysulfides generates a thiosulfate redox mediator, secures the intercalation pathway, and reveals Lewis acidic sites within the siloxene galleries. The 2DSi utilizes the corresponding in‐situ‐formed electrocatalyst, the 2D confinement effect of the layered structure, and the surface affinity based on Lewis acid–base interaction to improve the energy density of 2DSi‐based LSB cells. Combined with the commercial carbon‐based current collector, 2DSi‐based LSB cells achieve a volumetric energy density of 612 Wh Lcell−1 at 1 mA cm−2 with minor degradation of 0.17% per cycle, which rivals those of state‐of‐the‐art LSBs. This study presents a method for the industrial production of high‐energy‐dense LSBs. |
| format |
article |
| author |
Hui‐Ju Kang Jae‐Woo Park Hyun Jin Hwang Heejin Kim Kwang‐Suk Jang Xiulei Ji Hae Jin Kim Won Bin Im Young‐Si Jun |
| author_facet |
Hui‐Ju Kang Jae‐Woo Park Hyun Jin Hwang Heejin Kim Kwang‐Suk Jang Xiulei Ji Hae Jin Kim Won Bin Im Young‐Si Jun |
| author_sort |
Hui‐Ju Kang |
| title |
Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| title_short |
Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| title_full |
Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| title_fullStr |
Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| title_full_unstemmed |
Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| title_sort |
electrocatalytic and stoichiometric reactivity of 2d layered siloxene for high‐energy‐dense lithium–sulfur batteries |
| publisher |
Wiley |
| publishDate |
2021 |
| url |
https://doaj.org/article/73d9dccf92034b0aa0efea3838398d07 |
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