Direct Oxygen-Oxygen Cleavage through Optimizing Interatomic Distances in Dual Single-atom Electrocatalysts for Efficient Oxygen Reduction Reaction.

Xie, Y; Chen, X; Sun, K; Zhang, J; Lai, W-H; Liu, H; Wang, G

Direct Oxygen-Oxygen Cleavage through Optimizing Interatomic Distances in Dual Single-atom Electrocatalysts for Efficient Oxygen Reduction Reaction.

Xie, Y

Chen, X Sun, K Zhang, J

Lai, W-H Liu, H

Wang, G

Permalink

Publisher:: WILEY-V C H VERLAG GMBH
Publication Type:: Journal Article
Citation:: Angew Chem Int Ed Engl, 2023, 62, (17), pp. e202301833
Issue Date:: 2023-04-17

Open Access

Copyright Clearance Process

Recently Added
In Progress
Open Access

This item is open access.

Adobe PDF

Download Published versionAdobe PDF (7.07 MB)

View on publisher's site

View statistics

Full metadata record

Field	Value	Language
dc.contributor.author	Xie, Y https://orcid.org/0000-0002-0296-8862
dc.contributor.author	Chen, X
dc.contributor.author	Sun, K
dc.contributor.author	Zhang, J https://orcid.org/0000-0001-5476-0134
dc.contributor.author	Lai, W-H
dc.contributor.author	Liu, H https://orcid.org/0000-0003-0266-9472
dc.contributor.author	Wang, G https://orcid.org/0000-0003-4295-8578
dc.date.accessioned	2024-03-04T03:41:35Z
dc.date.available	2024-03-04T03:41:35Z
dc.date.issued	2023-04-17
dc.identifier.citation	Angew Chem Int Ed Engl, 2023, 62, (17), pp. e202301833
dc.identifier.issn	1433-7851
dc.identifier.issn	1521-3773
dc.identifier.uri	http://hdl.handle.net/10453/176057
dc.description.abstract	The oxygen reduction reaction (ORR) on transition single-atom catalysts (SACs) is sustainable in energy-conversion devices. However, the atomically controllable fabrication of single-atom sites and the sluggish kinetics of ORR have remained challenging. Here, we accelerate the kinetics of acid ORR through a direct O-O cleavage pathway through using a bi-functional ligand-assisted strategy to pre-control the distance of hetero-metal atoms. Concretely, the as-synthesized Fe-Zn diatomic pairs on carbon substrates exhibited an outstanding ORR performance with the ultrahigh half-wave potential of 0.86 V vs. RHE in acid electrolyte. Experimental evidence and density functional theory calculations confirmed that the Fe-Zn diatomic pairs with a specific distance range of around 3 Å, which is the key to their ultrahigh activity, average the interaction between hetero-diatomic active sites and oxygen molecules. This work offers new insight into atomically controllable SACs synthesis and addresses the limitations of the ORR dissociative mechanism.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	WILEY-V C H VERLAG GMBH
dc.relation	http://purl.org/au-research/grants/arc/FT180100705
dc.relation	http://purl.org/au-research/grants/arc/DP180102297
dc.relation	http://purl.org/au-research/grants/arc/IH180100020
dc.relation	http://purl.org/au-research/grants/arc/DP200101249
dc.relation	http://purl.org/au-research/grants/arc/DP210101389
dc.relation.ispartof	Angew Chem Int Ed Engl
dc.relation.isbasedon	10.1002/anie.202301833
dc.rights	info:eu-repo/semantics/openAccess
dc.subject	03 Chemical Sciences
dc.subject.classification	Organic Chemistry
dc.subject.classification	34 Chemical sciences
dc.title	Direct Oxygen-Oxygen Cleavage through Optimizing Interatomic Distances in Dual Single-atom Electrocatalysts for Efficient Oxygen Reduction Reaction.
dc.type	Journal Article
utslib.citation.volume	62
utslib.location.activity	Germany
utslib.for	03 Chemical Sciences
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	2024-03-04T03:41:32Z
pubs.issue	17
pubs.publication-status	Published
pubs.volume	62
utslib.citation.issue	17

Abstract:

The oxygen reduction reaction (ORR) on transition single-atom catalysts (SACs) is sustainable in energy-conversion devices. However, the atomically controllable fabrication of single-atom sites and the sluggish kinetics of ORR have remained challenging. Here, we accelerate the kinetics of acid ORR through a direct O-O cleavage pathway through using a bi-functional ligand-assisted strategy to pre-control the distance of hetero-metal atoms. Concretely, the as-synthesized Fe-Zn diatomic pairs on carbon substrates exhibited an outstanding ORR performance with the ultrahigh half-wave potential of 0.86 V vs. RHE in acid electrolyte. Experimental evidence and density functional theory calculations confirmed that the Fe-Zn diatomic pairs with a specific distance range of around 3 Å, which is the key to their ultrahigh activity, average the interaction between hetero-diatomic active sites and oxygen molecules. This work offers new insight into atomically controllable SACs synthesis and addresses the limitations of the ORR dissociative mechanism.

Please use this identifier to cite or link to this item:

http://hdl.handle.net/10453/176057