Enhanced Elastic Migration of Magnesium Cations in alpha-Manganese Dioxide Tunnels Locally Tuned by Aluminium Substitution

Ding, Y; Zhang, S; Li, J; Sun, Y; Yin, B; Li, H; Ma, Y; Wang, Z; Ge, H; Su, D; Ma, T

Enhanced Elastic Migration of Magnesium Cations in alpha-Manganese Dioxide Tunnels Locally Tuned by Aluminium Substitution

Ding, Y Zhang, S Li, J Sun, Y Yin, B Li, H Ma, Y Wang, Z Ge, H Su, D

Ma, T

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Publisher:: WILEY-V C H VERLAG GMBH
Publication Type:: Journal Article
Citation:: Advanced Functional Materials, 2023, 33, (2)
Issue Date:: 2023-01-10

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Field	Value	Language
dc.contributor.author	Ding, Y
dc.contributor.author	Zhang, S
dc.contributor.author	Li, J
dc.contributor.author	Sun, Y
dc.contributor.author	Yin, B
dc.contributor.author	Li, H
dc.contributor.author	Ma, Y
dc.contributor.author	Wang, Z
dc.contributor.author	Ge, H
dc.contributor.author	Su, D https://orcid.org/0000-0002-3972-8205
dc.contributor.author	Ma, T
dc.date.accessioned	2024-03-19T02:37:05Z
dc.date.available	2024-03-19T02:37:05Z
dc.date.issued	2023-01-10
dc.identifier.citation	Advanced Functional Materials, 2023, 33, (2)
dc.identifier.issn	1616-301X
dc.identifier.issn	1616-3028
dc.identifier.uri	http://hdl.handle.net/10453/176900
dc.description.abstract	The harsh conditions of large hydrated ion radius of Mg2+ cations and the strong electrostatic interaction with the host material put forward higher requirements for high-performance aqueous magnesium ion (Mg2+) energy storage devices. Herein, substituted aluminium ions (Al3+) doped α-MnO2 materials are prepared. The introduction of Al3+ cations adjust the local chemical environment inside the tunnel structure of α-MnO2 and precisely regulates the diffusion behavior of inserted Mg2+ cations. The shortened oxygens’ distance and abundant oxygen defects result in a substantially enhanced elastic migration pattern of Mg2+ cations driven by strengthened electrostatic attraction, which brings the lower diffusion energy barrier, improved reaction kinetics, and adaptive volume expansion as evidenced by Climbing Image-Nudged Elastic Band density function theory calculations coupled with experimental confirmation in X-ray photoelectron spectroscopy, electron paramagnetic resonance, and galvanostatic intermittent titration technique. As a result, this rationally designed cathode exhibits a high reversible capacity of 197.02 mAh g-1 at 0.1 A g-1 and stable cycle performance of 2500 cycles with 82% retention. These parameters are among the best of Mg-ion capacitors reported to date. This study offers a detailed insight into the local tunnel structure tunning effect and opens up a new path of modification for tunnel-type structural materials.
dc.language	English
dc.publisher	WILEY-V C H VERLAG GMBH
dc.relation.ispartof	Advanced Functional Materials
dc.relation.isbasedon	10.1002/adfm.202210519
dc.rights	info:eu-repo/semantics/openAccess
dc.subject	02 Physical Sciences, 03 Chemical Sciences, 09 Engineering
dc.subject.classification	Materials
dc.subject.classification	34 Chemical sciences
dc.subject.classification	40 Engineering
dc.subject.classification	51 Physical sciences
dc.title	Enhanced Elastic Migration of Magnesium Cations in alpha-Manganese Dioxide Tunnels Locally Tuned by Aluminium Substitution
dc.type	Journal Article
utslib.citation.volume	33
utslib.for	02 Physical Sciences
utslib.for	03 Chemical Sciences
utslib.for	09 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	open_access	*
dc.date.updated	2024-03-19T02:37:03Z
pubs.issue	2
pubs.publication-status	Published
pubs.volume	33
utslib.citation.issue	2

Abstract:

The harsh conditions of large hydrated ion radius of Mg2+ cations and the strong electrostatic interaction with the host material put forward higher requirements for high-performance aqueous magnesium ion (Mg2+) energy storage devices. Herein, substituted aluminium ions (Al3+) doped α-MnO2 materials are prepared. The introduction of Al3+ cations adjust the local chemical environment inside the tunnel structure of α-MnO2 and precisely regulates the diffusion behavior of inserted Mg2+ cations. The shortened oxygens’ distance and abundant oxygen defects result in a substantially enhanced elastic migration pattern of Mg2+ cations driven by strengthened electrostatic attraction, which brings the lower diffusion energy barrier, improved reaction kinetics, and adaptive volume expansion as evidenced by Climbing Image-Nudged Elastic Band density function theory calculations coupled with experimental confirmation in X-ray photoelectron spectroscopy, electron paramagnetic resonance, and galvanostatic intermittent titration technique. As a result, this rationally designed cathode exhibits a high reversible capacity of 197.02 mAh g-1 at 0.1 A g-1 and stable cycle performance of 2500 cycles with 82% retention. These parameters are among the best of Mg-ion capacitors reported to date. This study offers a detailed insight into the local tunnel structure tunning effect and opens up a new path of modification for tunnel-type structural materials.

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http://hdl.handle.net/10453/176900