Hybrid Molecular Sieve-Based Interfacial Layer with Physical Confinement and Desolvation Effect for Dendrite-free Zinc Metal Anodes.

Xu, J; Han, P; Jin, Y; Lu, H; Sun, B; Gao, B; He, T; Xu, X; Pinna, N; Wang, G

Hybrid Molecular Sieve-Based Interfacial Layer with Physical Confinement and Desolvation Effect for Dendrite-free Zinc Metal Anodes.

Xu, J Han, P Jin, Y Lu, H Sun, B

Gao, B He, T Xu, X

Pinna, N Wang, G

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Publisher:: AMER CHEMICAL SOC
Publication Type:: Journal Article
Citation:: ACS Nano, 2024, 18, (28), pp. 18592-18603
Issue Date:: 2024-07-16

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Field	Value	Language
dc.contributor.author	Xu, J
dc.contributor.author	Han, P
dc.contributor.author	Jin, Y
dc.contributor.author	Lu, H
dc.contributor.author	Sun, B https://orcid.org/0000-0002-4365-486X
dc.contributor.author	Gao, B
dc.contributor.author	He, T
dc.contributor.author	Xu, X https://orcid.org/0000-0002-2598-3766
dc.contributor.author	Pinna, N
dc.contributor.author	Wang, G https://orcid.org/0000-0003-4295-8578
dc.date.accessioned	2024-09-09T04:05:22Z
dc.date.available	2024-09-09T04:05:22Z
dc.date.issued	2024-07-16
dc.identifier.citation	ACS Nano, 2024, 18, (28), pp. 18592-18603
dc.identifier.issn	1936-0851
dc.identifier.issn	1936-086X
dc.identifier.uri	http://hdl.handle.net/10453/180754
dc.description.abstract	The side reactions and dendrite growth at the interface of Zn anodes greatly limit their practical applications in Zn metal batteries. Herein, we propose a hybrid molecular sieve-based interfacial layer (denoted as Z7M3) with a hierarchical porous structure for Zn metal anodes, which contains 70 vol % microporous ZSM-5 molecular sieves and 30 vol % mesoporous MCM-41 molecular sieves. Through comprehensive molecular dynamics simulations, we demonstrate that the mesopores (∼2.5 nm) of MCM-41 can limit the disordered diffusion of free water molecules and increase the wettability of the interfacial layer toward aqueous electrolytes. In addition, the micropores (∼0.56 nm) of ZSM-5 can optimize the Zn2+ solvation structures by reducing the bonded water molecules, which simultaneously decrease the constraint force of solvated water molecules to Zn2+ ions, thus promoting the penetrability and diffusion kinetics of Zn2+ ions in Z7M3. The synergetic effects from the hybrid molecular sieves maintain a constant Zn2+ concentration on the surface of the Zn electrode during Zn deposition, contributing to dendrite-free Zn anodes. Consequently, Z7M3-coated Zn electrodes achieved excellent cycling stability in both half and full cells.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	AMER CHEMICAL SOC
dc.relation	http://purl.org/au-research/grants/arc/DP210101389
dc.relation	http://purl.org/au-research/grants/arc/FT220100561
dc.relation	http://purl.org/au-research/grants/arc/DP230101579
dc.relation.ispartof	ACS Nano
dc.relation.isbasedon	10.1021/acsnano.4c04632
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject.classification	Nanoscience & Nanotechnology
dc.title	Hybrid Molecular Sieve-Based Interfacial Layer with Physical Confinement and Desolvation Effect for Dendrite-free Zinc Metal Anodes.
dc.type	Journal Article
utslib.citation.volume	18
utslib.location.activity	United States
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Engineering and Information Technology
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
pubs.organisational-group	University of Technology Sydney/Faculty of Engineering and Information Technology/School of Biomedical Engineering
pubs.organisational-group	University of Technology Sydney/All Manual Groups
pubs.organisational-group	University of Technology Sydney/All Manual Groups/Centre for Clean Energy Technology(CCET)
utslib.copyright.status	closed_access	*
dc.date.updated	2024-09-09T04:05:20Z
pubs.issue	28
pubs.publication-status	Published
pubs.volume	18
utslib.citation.issue	28

Abstract:

The side reactions and dendrite growth at the interface of Zn anodes greatly limit their practical applications in Zn metal batteries. Herein, we propose a hybrid molecular sieve-based interfacial layer (denoted as Z7M3) with a hierarchical porous structure for Zn metal anodes, which contains 70 vol % microporous ZSM-5 molecular sieves and 30 vol % mesoporous MCM-41 molecular sieves. Through comprehensive molecular dynamics simulations, we demonstrate that the mesopores (∼2.5 nm) of MCM-41 can limit the disordered diffusion of free water molecules and increase the wettability of the interfacial layer toward aqueous electrolytes. In addition, the micropores (∼0.56 nm) of ZSM-5 can optimize the Zn2+ solvation structures by reducing the bonded water molecules, which simultaneously decrease the constraint force of solvated water molecules to Zn2+ ions, thus promoting the penetrability and diffusion kinetics of Zn2+ ions in Z7M3. The synergetic effects from the hybrid molecular sieves maintain a constant Zn2+ concentration on the surface of the Zn electrode during Zn deposition, contributing to dendrite-free Zn anodes. Consequently, Z7M3-coated Zn electrodes achieved excellent cycling stability in both half and full cells.

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http://hdl.handle.net/10453/180754