Small molecule π-conjugated electron acceptor for highly enhanced photocatalytic nitrogen reduction of BiOBr

Hao, D; Ma, T; Jia, B; Wei, Y; Bai, X; Wei, W; Ni, BJ

Small molecule π-conjugated electron acceptor for highly enhanced photocatalytic nitrogen reduction of BiOBr

Hao, D Ma, T Jia, B Wei, Y Bai, X Wei, W

Ni, BJ

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Publisher:: JOURNAL MATER SCI TECHNOL
Publication Type:: Journal Article
Citation:: Journal of Materials Science and Technology, 2022, 109, pp. 276-281
Issue Date:: 2022-05-20

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Field	Value	Language
dc.contributor.author	Hao, D
dc.contributor.author	Ma, T
dc.contributor.author	Jia, B
dc.contributor.author	Wei, Y
dc.contributor.author	Bai, X
dc.contributor.author	Wei, W https://orcid.org/0000-0001-5613-337X
dc.contributor.author	Ni, BJ
dc.date.accessioned	2023-03-23T22:16:07Z
dc.date.available	2023-03-23T22:16:07Z
dc.date.issued	2022-05-20
dc.identifier.citation	Journal of Materials Science and Technology, 2022, 109, pp. 276-281
dc.identifier.issn	1005-0302
dc.identifier.uri	http://hdl.handle.net/10453/168245
dc.description.abstract	Artificial ammonia synthesis using solar energy is of great significance as it can help narrow the gap to the zero-net emission target. However, the current photocatalytic activity is generally too low for mass production. Herein, we report a novel bismuth bromide oxide (BiOBr)-Tetracyanoquinodimethane (TCNQ) photocatalyst prepared via a facile self-assembly method. Due to the well-match band structure of TCNQ and BiOBr, the separation and transfer of photogenerated electron-hole pairs were significantly boosted. More importantly, the abundant delocalized π electrons of TCNQ, and the electron-withdrawing property of TNCQ made electrons efficiently accumulated on the catalysts, which can strengthen the adsorption and cleavage of nitrogen molecules. As a result, the photocatalytic activity increased significantly. The highest ammonia yield of the optimized sample reached 2.617 mg/(h gcat), which was 5.6-fold as that of pristine BiOBr and higher than the reported BiOBr-based photocatalysts. The isotope labeled 15N2 was used to confirm that the ammonia is formed form the fixation of N2. Meanwhile, the sample also had good stability. After 4-time usage, the photocatalysts still had about 81.8% as the fresh sample. The results of this work provide a new way for optimizing the electronic structure of photocatalysts to achieve highly efficient photochemical N2 reduction.
dc.language	English
dc.publisher	JOURNAL MATER SCI TECHNOL
dc.relation.ispartof	Journal of Materials Science and Technology
dc.relation.isbasedon	10.1016/j.jmst.2021.08.085
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	0910 Manufacturing Engineering, 0912 Materials Engineering, 0913 Mechanical Engineering
dc.subject.classification	Materials
dc.title	Small molecule π-conjugated electron acceptor for highly enhanced photocatalytic nitrogen reduction of BiOBr
dc.type	Journal Article
utslib.citation.volume	109
utslib.for	0910 Manufacturing Engineering
utslib.for	0912 Materials Engineering
utslib.for	0913 Mechanical Engineering
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology
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/Strength - CTWW - Centre for Technology in Water and Wastewater Treatment
utslib.copyright.status	closed_access	*
dc.date.updated	2023-03-23T22:16:06Z
pubs.publication-status	Published
pubs.volume	109

Abstract:

Artificial ammonia synthesis using solar energy is of great significance as it can help narrow the gap to the zero-net emission target. However, the current photocatalytic activity is generally too low for mass production. Herein, we report a novel bismuth bromide oxide (BiOBr)-Tetracyanoquinodimethane (TCNQ) photocatalyst prepared via a facile self-assembly method. Due to the well-match band structure of TCNQ and BiOBr, the separation and transfer of photogenerated electron-hole pairs were significantly boosted. More importantly, the abundant delocalized π electrons of TCNQ, and the electron-withdrawing property of TNCQ made electrons efficiently accumulated on the catalysts, which can strengthen the adsorption and cleavage of nitrogen molecules. As a result, the photocatalytic activity increased significantly. The highest ammonia yield of the optimized sample reached 2.617 mg/(h gcat), which was 5.6-fold as that of pristine BiOBr and higher than the reported BiOBr-based photocatalysts. The isotope labeled 15N2 was used to confirm that the ammonia is formed form the fixation of N2. Meanwhile, the sample also had good stability. After 4-time usage, the photocatalysts still had about 81.8% as the fresh sample. The results of this work provide a new way for optimizing the electronic structure of photocatalysts to achieve highly efficient photochemical N2 reduction.

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http://hdl.handle.net/10453/168245