Dominant Polar Surfaces of Colloidal II-VI Wurtzite Semiconductor Nanocrystals Enabled by Cation Exchange.

Wang, A; Wang, W; Chen, J; Mao, R; Pang, Y; Li, Y; Chen, W; Chen, D; Hao, D; Ni, B-J; Saunders, M; Jia, G

Dominant Polar Surfaces of Colloidal II-VI Wurtzite Semiconductor Nanocrystals Enabled by Cation Exchange.

Wang, A Wang, W Chen, J Mao, R Pang, Y Li, Y Chen, W Chen, D Hao, D Ni, B-J Saunders, M Jia, G

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Publisher:: American Chemical Society
Publication Type:: Journal Article
Citation:: Journal of Physical Chemistry Letters, 2020, 11, (13), pp. 4990-4997
Issue Date:: 2020-07

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Field	Value	Language
dc.contributor.author	Wang, A
dc.contributor.author	Wang, W
dc.contributor.author	Chen, J
dc.contributor.author	Mao, R
dc.contributor.author	Pang, Y
dc.contributor.author	Li, Y
dc.contributor.author	Chen, W
dc.contributor.author	Chen, D
dc.contributor.author	Hao, D
dc.contributor.author	Ni, B-J
dc.contributor.author	Saunders, M
dc.contributor.author	Jia, G
dc.date.accessioned	2021-02-09T09:30:35Z
dc.date.available	2021-02-09T09:30:35Z
dc.date.issued	2020-07
dc.identifier.citation	Journal of Physical Chemistry Letters, 2020, 11, (13), pp. 4990-4997
dc.identifier.issn	1948-7185
dc.identifier.issn	1948-7185
dc.identifier.uri	http://hdl.handle.net/10453/145995
dc.description.abstract	Polar surfaces of ionic crystals are of growing technological importance, with implications for the efficiency of photocatalysts, gas sensors, and electronic devices. The creation of ionic nanocrystals with high percentages of polar surfaces is an option for improving their efficiency in the aforementioned applications but is hard to accomplish because they are less thermodynamically stable and prone to vanish during the growth process. Herein, we develop a strategy that is capable of producing polar surface-dominated II-VI semiconductor nanocrystals, including ZnS and CdS, from copper sulfide hexagonal nanoplates through cation exchange reactions. The obtained wurtzite ZnS hexagonal nanoplates have dominant {002} polar surfaces, occupying up to 97.8% of all surfaces. Density functional theory calculations reveal the polar surfaces can be stabilized by a charge transfer of 0.25 eV/formula from the anion-terminated surface to the cation-terminated surface, which also explains the presence of polar surfaces in the initial Cu1.75S hexagonal nanoplates with cation deficiency prior to cation exchange reactions. Experimental results showed that the HER activity could be boosted by the surface polarization of polar surface-dominated ZnS hexagonal nanoplates. We anticipate this strategy is general and could be used with other systems to prepare nanocrystals with dominant polar surfaces. Furthermore, the availability of colloidal semiconductor nanocrystals with dominant polar surfaces produced through this strategy opens a new avenue for improving their efficiency in catalysis, photocatalysis, gas sensing, and other applications.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	American Chemical Society
dc.relation.ispartof	Journal of Physical Chemistry Letters
dc.relation.isbasedon	http://dx.doi.org/10.1021/acs.jpclett.0c01372
dc.rights	info:eu-repo/semantics/restrictedAccess
dc.subject	02 Physical Sciences, 03 Chemical Sciences
dc.title	Dominant Polar Surfaces of Colloidal II-VI Wurtzite Semiconductor Nanocrystals Enabled by Cation Exchange.
dc.type	Journal Article
utslib.citation.volume	11
utslib.location.activity	United States
utslib.for	02 Physical Sciences
utslib.for	03 Chemical Sciences
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology
pubs.organisational-group	/University of Technology Sydney/Strength - CTWW - Centre for Technology in Water and Wastewater Treatment
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology/School of Civil and Environmental Engineering
pubs.organisational-group	/University of Technology Sydney
utslib.copyright.status	closed_access	*
pubs.consider-herdc	true
dc.date.updated	2021-02-09T09:30:26Z
pubs.issue	13
pubs.publication-status	Published
pubs.volume	11
utslib.citation.issue	13

Abstract:

Polar surfaces of ionic crystals are of growing technological importance, with implications for the efficiency of photocatalysts, gas sensors, and electronic devices. The creation of ionic nanocrystals with high percentages of polar surfaces is an option for improving their efficiency in the aforementioned applications but is hard to accomplish because they are less thermodynamically stable and prone to vanish during the growth process. Herein, we develop a strategy that is capable of producing polar surface-dominated II-VI semiconductor nanocrystals, including ZnS and CdS, from copper sulfide hexagonal nanoplates through cation exchange reactions. The obtained wurtzite ZnS hexagonal nanoplates have dominant {002} polar surfaces, occupying up to 97.8% of all surfaces. Density functional theory calculations reveal the polar surfaces can be stabilized by a charge transfer of 0.25 eV/formula from the anion-terminated surface to the cation-terminated surface, which also explains the presence of polar surfaces in the initial Cu1.75S hexagonal nanoplates with cation deficiency prior to cation exchange reactions. Experimental results showed that the HER activity could be boosted by the surface polarization of polar surface-dominated ZnS hexagonal nanoplates. We anticipate this strategy is general and could be used with other systems to prepare nanocrystals with dominant polar surfaces. Furthermore, the availability of colloidal semiconductor nanocrystals with dominant polar surfaces produced through this strategy opens a new avenue for improving their efficiency in catalysis, photocatalysis, gas sensing, and other applications.

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http://hdl.handle.net/10453/145995