MXene (Ti <inf>3</inf> C <inf>2</inf> ) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO <inf>2</inf>

Zhao, D; Chen, Z; Yang, W; Liu, S; Zhang, X; Yu, Y; Cheong, WC; Zheng, L; Ren, F; Ying, G; Cao, X; Wang, D; Peng, Q; Wang, G; Chen, C

MXene (Ti <inf>3</inf> C <inf>2</inf> ) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO <inf>2</inf>

Zhao, D Chen, Z Yang, W Liu, S Zhang, X Yu, Y Cheong, WC Zheng, L Ren, F Ying, G Cao, X Wang, D Peng, Q Wang, G

Chen, C

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Publication Type:: Journal Article
Citation:: Journal of the American Chemical Society, 2019, 141 (9), pp. 4086 - 4093
Issue Date:: 2019-03-06

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Field	Value	Language
dc.contributor.author	Zhao, D	en_US
dc.contributor.author	Chen, Z	en_US
dc.contributor.author	Yang, W	en_US
dc.contributor.author	Liu, S	en_US
dc.contributor.author	Zhang, X	en_US
dc.contributor.author	Yu, Y	en_US
dc.contributor.author	Cheong, WC	en_US
dc.contributor.author	Zheng, L	en_US
dc.contributor.author	Ren, F	en_US
dc.contributor.author	Ying, G	en_US
dc.contributor.author	Cao, X	en_US
dc.contributor.author	Wang, D	en_US
dc.contributor.author	Peng, Q	en_US
dc.contributor.author	Wang, G https://orcid.org/0000-0003-4295-8578	en_US
dc.contributor.author	Chen, C	en_US
dc.date.issued	2019-03-06	en_US
dc.identifier.citation	Journal of the American Chemical Society, 2019, 141 (9), pp. 4086 - 4093	en_US
dc.identifier.issn	0002-7863	en_US
dc.identifier.uri	http://hdl.handle.net/10453/136125
dc.description.abstract	© Copyright 2019 American Chemical Society. A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report the preparation of stabilized single-atom catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti 3-x C 2 T y MXene nanosheets characterized by abundant Ti-deficit vacancy defects and a high reducing capability. The single atoms therein form strong metal-carbon bonds with the Ti 3-x C 2 T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt 1 /Ti 3-x C 2 T y offers a green route to utilizing greenhouse gas CO 2 , via the formylation of amines, as a C 1 source in organic synthesis. DFT calculations reveal that, compared to Pt nanoparticles, the single Pt atoms on Ti 3-x C 2 T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO 2 , and aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities for the fabrication of SACs and the applications of MXenes in organic synthesis.	en_US
dc.relation.ispartof	Journal of the American Chemical Society	en_US
dc.relation.isbasedon	10.1021/jacs.8b13579	en_US
dc.subject.classification	General Chemistry	en_US
dc.title	MXene (Ti <inf>3</inf> C <inf>2</inf> ) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO <inf>2</inf>	en_US
dc.type	Journal Article
utslib.citation.volume	9	en_US
utslib.citation.volume	141	en_US
utslib.for	0306 Physical Chemistry (incl. Structural)	en_US
utslib.for	03 Chemical Sciences	en_US
pubs.embargo.period	Not known	en_US
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
pubs.issue	9	en_US
pubs.publication-status	Published	en_US
pubs.volume	141	en_US

Abstract:

© Copyright 2019 American Chemical Society. A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report the preparation of stabilized single-atom catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti 3-x C 2 T y MXene nanosheets characterized by abundant Ti-deficit vacancy defects and a high reducing capability. The single atoms therein form strong metal-carbon bonds with the Ti 3-x C 2 T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt 1 /Ti 3-x C 2 T y offers a green route to utilizing greenhouse gas CO 2 , via the formylation of amines, as a C 1 source in organic synthesis. DFT calculations reveal that, compared to Pt nanoparticles, the single Pt atoms on Ti 3-x C 2 T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO 2 , and aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities for the fabrication of SACs and the applications of MXenes in organic synthesis.

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http://hdl.handle.net/10453/136125