Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis.

Huo, J; Cao, X; Tian, Y; Li, L; Qu, J; Xie, Y; Nie, X; Zhao, Y; Zhang, J; Liu, H

Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis.

Huo, J Cao, X Tian, Y Li, L Qu, J Xie, Y

Nie, X Zhao, Y

Zhang, J

Liu, H

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Publisher:: ROYAL SOC CHEMISTRY
Publication Type:: Journal Article
Citation:: Nanoscale, 2023, 15, (11), pp. 5448-5457
Issue Date:: 2023-03-16

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Field	Value	Language
dc.contributor.author	Huo, J
dc.contributor.author	Cao, X
dc.contributor.author	Tian, Y
dc.contributor.author	Li, L
dc.contributor.author	Qu, J
dc.contributor.author	Xie, Y https://orcid.org/0000-0002-0296-8862
dc.contributor.author	Nie, X
dc.contributor.author	Zhao, Y https://orcid.org/0000-0002-5325-8991
dc.contributor.author	Zhang, J https://orcid.org/0000-0001-5476-0134
dc.contributor.author	Liu, H https://orcid.org/0000-0003-0266-9472
dc.date.accessioned	2024-02-13T22:51:00Z
dc.date.available	2024-02-13T22:51:00Z
dc.date.issued	2023-03-16
dc.identifier.citation	Nanoscale, 2023, 15, (11), pp. 5448-5457
dc.identifier.issn	2040-3364
dc.identifier.issn	2040-3372
dc.identifier.uri	http://hdl.handle.net/10453/175654
dc.description.abstract	Developing efficient and robust catalysts to replace Pt group metals for the oxygen reduction reaction (ORR) is conducive to achieving highly efficient energy conversion. Here, we develop a general ion exchange strategy to construct highly efficient ORR catalysts consisting of various atomically dispersed metal atoms anchored on N-doped porous carbon (M-SAs/NC) to investigate the atomic structure-catalytic activity relationship. The structure characterization results demonstrated that the achieved atomic structure varied due to the presence of different metal centers. Mn-SAs/NC consists of MnN3O1 centers, in which the Mn single atoms are stabilized by 3 N and 1 O. In contrast, the center metals in Fe-/Co-/Cu single-atom catalysts are coordinated by merely N atoms. Mn-SAs/NC delivers superior performance for the ORR with a half-wave potential (E1/2) of 0.91 V vs. RHE in 0.1 M KOH solution, outperforming that of the commercial Pt/C catalyst and the control Fe-/Co-/Cu single-atom catalysts. Furthermore, Mn-SAs/NC also shows excellent methanol tolerance and stability up to 5000 cycles. Density functional theory (DFT) calculations reveal that Mn single atom catalysts with MnN3O1 centers contributed to the superior ORR performance with lower energy barriers and optimized adsorption capacity of intermediates. These findings provide insights into the design and development of specific coordinated structures of atomically dispersed catalysts to facilitate the practical applications of energy conversion.
dc.format	Electronic
dc.language	eng
dc.publisher	ROYAL SOC CHEMISTRY
dc.relation.ispartof	Nanoscale
dc.relation.isbasedon	10.1039/d2nr06096e
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	02 Physical Sciences, 03 Chemical Sciences, 10 Technology
dc.subject.classification	Nanoscience & Nanotechnology
dc.subject.classification	34 Chemical sciences
dc.subject.classification	40 Engineering
dc.subject.classification	51 Physical sciences
dc.title	Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis.
dc.type	Journal Article
utslib.citation.volume	15
utslib.location.activity	England
utslib.for	02 Physical Sciences
utslib.for	03 Chemical Sciences
utslib.for	10 Technology
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	2024-02-13T22:50:58Z
pubs.issue	11
pubs.publication-status	Published online
pubs.volume	15
utslib.citation.issue	11

Abstract:

Developing efficient and robust catalysts to replace Pt group metals for the oxygen reduction reaction (ORR) is conducive to achieving highly efficient energy conversion. Here, we develop a general ion exchange strategy to construct highly efficient ORR catalysts consisting of various atomically dispersed metal atoms anchored on N-doped porous carbon (M-SAs/NC) to investigate the atomic structure-catalytic activity relationship. The structure characterization results demonstrated that the achieved atomic structure varied due to the presence of different metal centers. Mn-SAs/NC consists of MnN3O1 centers, in which the Mn single atoms are stabilized by 3 N and 1 O. In contrast, the center metals in Fe-/Co-/Cu single-atom catalysts are coordinated by merely N atoms. Mn-SAs/NC delivers superior performance for the ORR with a half-wave potential (E1/2) of 0.91 V vs. RHE in 0.1 M KOH solution, outperforming that of the commercial Pt/C catalyst and the control Fe-/Co-/Cu single-atom catalysts. Furthermore, Mn-SAs/NC also shows excellent methanol tolerance and stability up to 5000 cycles. Density functional theory (DFT) calculations reveal that Mn single atom catalysts with MnN3O1 centers contributed to the superior ORR performance with lower energy barriers and optimized adsorption capacity of intermediates. These findings provide insights into the design and development of specific coordinated structures of atomically dispersed catalysts to facilitate the practical applications of energy conversion.

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http://hdl.handle.net/10453/175654