High volumetric energy density Li-S batteries enabled by dense sulfur monolith cathodes with ultra-small-sized sulfur immobilizers

Huang, Ying; Wang, Wei; Shan, Jiongwei; Zhu, Junlu; Wu, Shangyou; Li, Fen; Liu, Zhonggang; Li, Yunyong

doi:10.1016/j.cej.2020.126076

Cited by 37 publications

(17 citation statements)

References 55 publications

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“…[24] Huang et al reported a S/TiO 2 QDs/N-rich graphene that had a good cycling stability with an initial capacity of 1173 mAh g −1 . [25] Furthermore, Gao's group prepared a flexible TiO 2 QDs@MXene/S cathode in which the 2D transition metal nitrides and carbides increased the conductivity and alleviated the volumetric expansion. [26] Despite those achievements, the development of emerging cathodes with QDs for high-performance Li-S batteries, and establishing a general and well-controllable preparation approach, remain a challenge.…”

Section: Introductionmentioning

confidence: 99%

A Polysulfides‐Confined All‐in‐One Porous Microcapsule Lithium–Sulfur Battery Cathode

Liu

Zhu

Shen

et al. 2021

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Developing emerging materials for high energy‐density lithium–sulfur (Li–S) batteries is of great significance to suppress the shuttle effect of polysulfides and to accommodate the volumetric change of sulfur. Here, a novel porous microcapsule system containing a carbon nanotubes/tin dioxide quantum dots/S (CNTs/QDs/S) composite core and a porous shell prepared through a liquid‐driven coaxial microfluidic method as Li–S battery cathode is developed. The encapsulated CNTs in the microcapsules provide pathways for electron transport; SnO2 QDs on CNTs immobilize the polysulfides by strong adsorption, which is verified by using density functional theory calculations on binding energies. The porous shell of the microcapsule is beneficial for ion diffusion and electrolyte penetration. The void inside the microcapsule accommodates the volumetric change of sulfur. The Li–S battery based on the porous CNTs/QDs/S microcapsules displays a high capacity of 1025 mAh g−1 after 100 cycles at 0.1 C. When the sulfur loading is 2.03 mg cm−2, the battery shows a stable cycling life of 700 cycles, a Coulombic efficiency exceeding 99.9%, a recoverable rate‐performance during repeated tests, and a good temperature tolerance at both −5 and 45 °C, which indicates a potential for applications at different conditions.

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Section: Introductionmentioning

confidence: 99%

A Polysulfides‐Confined All‐in‐One Porous Microcapsule Lithium–Sulfur Battery Cathode

Liu

Zhu

Shen

et al. 2021

Small

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“…The absorption ability of all samples for Li 2 S 6 was also evaluated using UV–vis spectroscopy. For Li 2 S 6 in dimethyl ether, the band at 263 nm linked to S 6 2– indicates the presence of LiPSs. , Also, the order of the peak intensities of the solution containing the host and Li 2 S 6 is as follow: NbN-NW@C-800 > NbN-NW@C-1500 ≥ NbN-NW@C-500 > NbN-NW@Super P-75% > NbN-NW > pure Li 2 S 6 solution. This result means that more polysulfides are absorbed by NbN-NW@C-800, and the shuttle effect is effectively suppressed. ,, The XPS results are shown in Figure b,c, and two new peaks at 203.9/206.5 eV are assigned to the Nb–S species that appears in the Nb 3d XPS spectrum of NbN-NW@C-800 .…”

Section: Resultsmentioning

confidence: 75%

Mesoporous Niobium Nitride Nanowires Encapsulated in Carbon for High-Performance Lithium–Sulfur Batteries

Jia

Wang

et al. 2021

ACS Appl. Nano Mater.

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The shuttle effect of lithium polysulfides (LiPSs) is a fundamental problem restricting the commercialization of lithium–sulfur batteries. A polar conductive substrate serving as the sulfur positive host is proven to be an excellent strategy for the efficient immobilization and rapid conversion of LiPSs. Herein, a heterostructure material of niobium nitride nanowires encapsulated in carbon (NbN-NW@C) as a positive host for the sulfur cathode was designed and investigated. First-principles calculation confirms the existence of a strong chemical interaction between NbN-NW and LiPSs, which catalytically promotes the mutual conversion of LiPSs and insoluble Li2S/Li2S2, thus enhancing the redox reaction kinetics. The carbon layer with an adjustable thickness effectively improves the adsorption capacity of the host for LiPSs, and N2 adsorption–desorption shows that the maximum specific surface area of NbN-NW@C-800 is 81.0 m2 g–1. Besides, the metallic property of NbN-NW facilitates electron transmission and improves sulfur utilization. Benefiting from the rational design of the electrode structure, the cathode exhibits excellent cycle stability (the capacity retention is 81.8% after 100 cycles) and rate properties (783 mAh g–1 at 1 C).

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“…[1,2] LiÀ S battery is one of the promising candidates for the next-generation energy storage systems due to its high theoretical energy density (2600 Wh kg À 1 ), theoretical specific capacity (1675 mAh g À 1 ), environmental friendliness, low cost and earth-abundance sulfur material. [3][4][5][6] However, there are still multiple obstacles leading to poor cycle stability and rate performance, which inhibits the commercialization of LiÀ S battery. [7,8] They are mainly reflected in the following aspects: i) the inherent insulation of sulfur cathode and its reduction products Li 2 S/Li 2 S 2 , which induces low electron transport rate and the utilization of the sulfur species.…”

Section: Introductionmentioning

confidence: 99%

A Heterostructured Sulfonated CNT/Sulfur/CNT Cathode for Promoting the Binary Conversion of Polysulfides in Lithium‐Metal Batteries

Zhou

Liu

et al. 2021

Batteries & Supercaps

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The shuttle effect of lithium polysulfides (LiPS) and sluggish redox kinetics hinder the commercialization of lithium-sulfur (LiÀ S) batteries. Herein, we design a lightweight and multifunctional multi-walled carbon nanotube (CNT)/sulfur/lithiated sulfonated CNT (M/S/M-SO 3 Li) electrode as energy storage devices. Flexible CNT films ensure continuously electron/ion transmission and serve as LiPS shielding layer. Moreover, guided by DFT and experimental results, SO 3 groups exert a vital adsorption effect toward sulfur species but not NH 4 + groups.The SO 3 groups can not only employ as LiPS immobilizer by LiÀ O bands between LiPS and SO 3 , but also serve as multifunctional electrocatalyst to propel LiPS conversion via generating thiosulfate and polythionate and Li 2 S decomposition by reducing reaction overpotential. As expected, M/S/M-SO 3 Li electrode exhibits prominent rate capability (723.5 mAh g À 1 at 5 C), high sulfur loading (7.09 mAh cm À 2 at 5.0 mg cm À 2 sulfur), favorable anti-self-discharge capabilities (rest for 72 h at 0.5 C with 2.17 %).

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High volumetric energy density Li-S batteries enabled by dense sulfur monolith cathodes with ultra-small-sized sulfur immobilizers

Cited by 37 publications

References 55 publications

A Polysulfides‐Confined All‐in‐One Porous Microcapsule Lithium–Sulfur Battery Cathode

A Polysulfides‐Confined All‐in‐One Porous Microcapsule Lithium–Sulfur Battery Cathode

Mesoporous Niobium Nitride Nanowires Encapsulated in Carbon for High-Performance Lithium–Sulfur Batteries

A Heterostructured Sulfonated CNT/Sulfur/CNT Cathode for Promoting the Binary Conversion of Polysulfides in Lithium‐Metal Batteries

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