Blocking polysulfides with a Janus Fe<inf>3</inf>C/N-CNF@RGO electrodeviaphysiochemical confinement and catalytic conversion for high-performance lithium-sulfur batteries

Li, J; Zhang, H; Luo, L; Li, H; He, J; Zu, H; Liu, L; Liu, H; Wang, F; Song, J

Blocking polysulfides with a Janus Fe<inf>3</inf>C/N-CNF@RGO electrodeviaphysiochemical confinement and catalytic conversion for high-performance lithium-sulfur batteries

Li, J Zhang, H Luo, L Li, H He, J Zu, H Liu, L Liu, H

Wang, F Song, J

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Publisher:: ROYAL SOC CHEMISTRY
Publication Type:: Journal Article
Citation:: Journal of Materials Chemistry A, 2021, 9, (4), pp. 2205-2213
Issue Date:: 2021-01-28

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Field	Value	Language
dc.contributor.author	Li, J
dc.contributor.author	Zhang, H
dc.contributor.author	Luo, L
dc.contributor.author	Li, H
dc.contributor.author	He, J
dc.contributor.author	Zu, H
dc.contributor.author	Liu, L
dc.contributor.author	Liu, H https://orcid.org/0000-0003-0266-9472
dc.contributor.author	Wang, F
dc.contributor.author	Song, J
dc.date.accessioned	2022-01-17T03:40:09Z
dc.date.available	2022-01-17T03:40:09Z
dc.date.issued	2021-01-28
dc.identifier.citation	Journal of Materials Chemistry A, 2021, 9, (4), pp. 2205-2213
dc.identifier.issn	2050-7488
dc.identifier.issn	2050-7496
dc.identifier.uri	http://hdl.handle.net/10453/153206
dc.description.abstract	Lithium-sulfur batteries (LSBs) have shown great potential for application in high-density energy storage systems. However, the performance of LSBs is severely hindered by the shuttle effect and the sluggish reaction kinetics of lithium polysulfides (LiPSs). Here, a Janus Fe3C/N-CNF@RGO electrode consisting of a 1D Fe3C-decorated N-doped carbon nanofibers (Fe3C/N-CNFs) side and a 2D reduced graphene oxide (RGO) side was applied as a free-standing carrier for the Li2S6catholyte to improve the overall electrochemical performance of LSBs. The Fe3C/N-CNF layer endows the cathode with strong chemisorption abilities for LiPSs and accelerated the redox kineticsviacatalyzing the conversion of LiPSs. The 2D RGO sheets serve as a microscopic physical barrier and further resist the shuttling of LiPSs. Like a hunter's trap, behind the trap lies a net. Moreover, the 3D hierarchical conductive network based on 1D N-CNF and 2D RGO sheets enables fast electron transfer. Based on the synergetic effects of chemical immobilization, catalytic abilities, and a physical barrier in a 3D conductive network, LSBs with optimal Fe3C/N-CNF@RGO electrodes exhibit robust long-term cycling stability (a decay rate of only 0.0089% per cycle at 0.5C for 300 cycles), superior rate capabilities (821.7 mA h g−1at 2.0C), and stable cycling performance at high sulfur loading (6.29 mg cm−2). This work defines an emerging viewpoint relating to the design of novel sulfur carriers with multiple synergistic effects for application in LSBs.
dc.language	English
dc.publisher	ROYAL SOC CHEMISTRY
dc.relation.ispartof	Journal of Materials Chemistry A
dc.relation.isbasedon	10.1039/d0ta10515e
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	0303 Macromolecular and Materials Chemistry, 0912 Materials Engineering, 0915 Interdisciplinary Engineering
dc.title	Blocking polysulfides with a Janus Fe<inf>3</inf>C/N-CNF@RGO electrodeviaphysiochemical confinement and catalytic conversion for high-performance lithium-sulfur batteries
dc.type	Journal Article
utslib.citation.volume	9
utslib.for	0303 Macromolecular and Materials Chemistry
utslib.for	0912 Materials Engineering
utslib.for	0915 Interdisciplinary Engineering
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Science
pubs.organisational-group	/University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
pubs.organisational-group	/University of Technology Sydney/Strength - CCET - Centre for Clean Energy Technology
utslib.copyright.status	closed_access	*
dc.date.updated	2022-01-17T03:40:08Z
pubs.issue	4
pubs.publication-status	Published
pubs.volume	9
utslib.citation.issue	4

Abstract:

Lithium-sulfur batteries (LSBs) have shown great potential for application in high-density energy storage systems. However, the performance of LSBs is severely hindered by the shuttle effect and the sluggish reaction kinetics of lithium polysulfides (LiPSs). Here, a Janus Fe3C/N-CNF@RGO electrode consisting of a 1D Fe3C-decorated N-doped carbon nanofibers (Fe3C/N-CNFs) side and a 2D reduced graphene oxide (RGO) side was applied as a free-standing carrier for the Li2S6catholyte to improve the overall electrochemical performance of LSBs. The Fe3C/N-CNF layer endows the cathode with strong chemisorption abilities for LiPSs and accelerated the redox kineticsviacatalyzing the conversion of LiPSs. The 2D RGO sheets serve as a microscopic physical barrier and further resist the shuttling of LiPSs. Like a hunter's trap, behind the trap lies a net. Moreover, the 3D hierarchical conductive network based on 1D N-CNF and 2D RGO sheets enables fast electron transfer. Based on the synergetic effects of chemical immobilization, catalytic abilities, and a physical barrier in a 3D conductive network, LSBs with optimal Fe3C/N-CNF@RGO electrodes exhibit robust long-term cycling stability (a decay rate of only 0.0089% per cycle at 0.5C for 300 cycles), superior rate capabilities (821.7 mA h g−1at 2.0C), and stable cycling performance at high sulfur loading (6.29 mg cm−2). This work defines an emerging viewpoint relating to the design of novel sulfur carriers with multiple synergistic effects for application in LSBs.

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