In-situ exfoliation of porous carbon nitride nanosheets for enhanced hydrogen evolution

Gao, X; Feng, J; Su, D; Ma, Y; Wang, G; Ma, H; Zhang, J

In-situ exfoliation of porous carbon nitride nanosheets for enhanced hydrogen evolution

Gao, X Feng, J Su, D

Ma, Y Wang, G

Ma, H Zhang, J

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Publication Type:: Journal Article
Citation:: Nano Energy, 2019, 59 pp. 598 - 609
Issue Date:: 2019-05-01

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Field	Value	Language
dc.contributor.author	Gao, X	en_US
dc.contributor.author	Feng, J	en_US
dc.contributor.author	Su, D https://orcid.org/0000-0002-3972-8205	en_US
dc.contributor.author	Ma, Y	en_US
dc.contributor.author	Wang, G https://orcid.org/0000-0003-4295-8578	en_US
dc.contributor.author	Ma, H	en_US
dc.contributor.author	Zhang, J	en_US
dc.date.issued	2019-05-01	en_US
dc.identifier.citation	Nano Energy, 2019, 59 pp. 598 - 609	en_US
dc.identifier.issn	2211-2855	en_US
dc.identifier.uri	http://hdl.handle.net/10453/135532
dc.description.abstract	© 2019 Elsevier Ltd The development of water splitting technology is severely impeded by the limited strategies for preparing efficient photocatalyst with optimal structure. Herein, a facile structure and doping engineering strategy is proposed to obtain the atomic-thin mesoporous graphite carbon nitride (g-C 3 N 4 ) nanosheets with a large specific surface area of 212.5 m 2 g −1 , an ultra-large pore volume of 1.55 cm 3 g −1 , high C and O contents of ∼51.4 and 4.8% via an acid-assisted exfoliation route without any hard templates. The theoretical calculation reveals that the introduction of additional C/O atoms into g-C 3 N 4 matrix would boost the charge transfer rate and charge separation efficiency due to the enhanced electronic polarization effect (Bader Charge) and shortened bond lengths. Additionally, the electronic conductivity is demonstrated to be enhanced due to the formation of delocalized π-bonding both experimentally and theoretically. The synergic contribution of textural and electronic features renders an excellent photoelectrochemical (PEC) performance with 50–60 times larger photocurrent in comparison with the pristine g-C 3 N 4 and high hydrogen evolution rates of 830.1 and 115.5 μmol g −1 h −1 under the solar- and visible-light irradiation, respectively. This in-situ exfoliation approach demonstrates a facile yet efficient method to synthesize highly porous carbon nitride materials with optimal structure and composition for efficient water splitting.	en_US
dc.relation	http://purl.org/au-research/grants/arc/DE170101009
dc.relation	http://purl.org/au-research/grants/arc/DP170100436
dc.relation.ispartof	Nano Energy	en_US
dc.relation.isbasedon	10.1016/j.nanoen.2019.03.016	en_US
dc.title	In-situ exfoliation of porous carbon nitride nanosheets for enhanced hydrogen evolution	en_US
dc.type	Journal Article
utslib.citation.volume	59	en_US
utslib.for	1007 Nanotechnology	en_US
utslib.for	0912 Materials Engineering	en_US
utslib.for	0303 Macromolecular and Materials Chemistry	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
pubs.organisational-group	/University of Technology Sydney/Students
utslib.copyright.status	closed_access
pubs.publication-status	Published	en_US
pubs.volume	59	en_US

Abstract:

© 2019 Elsevier Ltd The development of water splitting technology is severely impeded by the limited strategies for preparing efficient photocatalyst with optimal structure. Herein, a facile structure and doping engineering strategy is proposed to obtain the atomic-thin mesoporous graphite carbon nitride (g-C 3 N 4 ) nanosheets with a large specific surface area of 212.5 m 2 g −1 , an ultra-large pore volume of 1.55 cm 3 g −1 , high C and O contents of ∼51.4 and 4.8% via an acid-assisted exfoliation route without any hard templates. The theoretical calculation reveals that the introduction of additional C/O atoms into g-C 3 N 4 matrix would boost the charge transfer rate and charge separation efficiency due to the enhanced electronic polarization effect (Bader Charge) and shortened bond lengths. Additionally, the electronic conductivity is demonstrated to be enhanced due to the formation of delocalized π-bonding both experimentally and theoretically. The synergic contribution of textural and electronic features renders an excellent photoelectrochemical (PEC) performance with 50–60 times larger photocurrent in comparison with the pristine g-C 3 N 4 and high hydrogen evolution rates of 830.1 and 115.5 μmol g −1 h −1 under the solar- and visible-light irradiation, respectively. This in-situ exfoliation approach demonstrates a facile yet efficient method to synthesize highly porous carbon nitride materials with optimal structure and composition for efficient water splitting.

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http://hdl.handle.net/10453/135532