Optimizing the Carbon Dioxide Reduction Pathway through Surface Modification by Halogenation.

Liu, Z; Jiang, W; Liu, Z; Wang, Y; Wang, D; Hao, D; Yao, W; Teng, F

Optimizing the Carbon Dioxide Reduction Pathway through Surface Modification by Halogenation.

Liu, Z Jiang, W Liu, Z Wang, Y Wang, D Hao, D Yao, W Teng, F

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Publisher:: WILEY-V C H VERLAG GMBH
Publication Type:: Journal Article
Citation:: ChemSusChem, 2020, 13, (21), pp. 5638-5646
Issue Date:: 2020-11

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Field	Value	Language
dc.contributor.author	Liu, Z
dc.contributor.author	Jiang, W
dc.contributor.author	Liu, Z
dc.contributor.author	Wang, Y
dc.contributor.author	Wang, D
dc.contributor.author	Hao, D
dc.contributor.author	Yao, W
dc.contributor.author	Teng, F
dc.date.accessioned	2021-03-24T19:29:02Z
dc.date.available	2021-03-24T19:29:02Z
dc.date.issued	2020-11
dc.identifier.citation	ChemSusChem, 2020, 13, (21), pp. 5638-5646
dc.identifier.issn	1864-5631
dc.identifier.issn	1864-564X
dc.identifier.uri	http://hdl.handle.net/10453/147507
dc.description.abstract	Facilitating the charge separation of semiconductor photocatalysts to increase the photocatalytic CO<sub>2</sub> reduction activity has become a great challenge for sustainable energy conversion. Herein, the surface halogen-modified defect-rich Bi<sub>2</sub> WO<sub>6</sub> nanosheets have been successfully prepared to address the aforementioned challenge. Importantly, the modification of surface with halogen atoms is beneficial for the adsorption and activation for CO<sub>2</sub> molecules and charge separation. These properties have been analyzed by experimental and theoretical methods. DFT calculations revealed that the modification of the Bi<sub>2</sub> WO<sub>6</sub> surface with Br atoms can decrease the formation energy of the *COOH intermediate, which accelerates CO<sub>2</sub> conversion. All halogen-modified defect-rich Bi<sub>2</sub> WO<sub>6</sub> nanosheets showed an enhanced photocatalytic CO<sub>2</sub> reduction activity. Specifically, Br-Bi<sub>2</sub> WO<sub>6</sub> exhibited the best CO generation rate of 13.8 μmol g<sup>-1</sup> h<sup>-1</sup> , which is roughly 7.3 times as high as the unmodified defect-rich Bi<sub>2</sub> WO<sub>6</sub> (1.9 μmol g<sup>-1</sup> h<sup>-1</sup> ). Moreover, in the presence of a cocatalyst (cobalt phthalocyanine) and a sacrificial agent (triethanolamine), Br-Bi<sub>2</sub> WO<sub>6</sub> exhibited an even further improved CO generation rate of 187 μmol g<sup>-1</sup> h<sup>-1</sup> . This finding provides a new approach to optimize the CO<sub>2</sub> reduction pathway of semiconductor photocatalysts, which is beneficial to develop highly efficient CO<sub>2</sub> reduction photocatalysts.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	WILEY-V C H VERLAG GMBH
dc.relation.ispartof	ChemSusChem
dc.relation.isbasedon	10.1002/cssc.202001855
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	0301 Analytical Chemistry, 0399 Other Chemical Sciences, 0904 Chemical Engineering
dc.subject.classification	General Chemistry
dc.subject.classification	Organic Chemistry
dc.title	Optimizing the Carbon Dioxide Reduction Pathway through Surface Modification by Halogenation.
dc.type	Journal Article
utslib.citation.volume	13
utslib.location.activity	Germany
utslib.for	0904 Chemical Engineering
utslib.for	0301 Analytical Chemistry
utslib.for	0399 Other Chemical Sciences
utslib.for	0904 Chemical 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
utslib.copyright.status	closed_access	*
dc.date.updated	2021-03-24T19:29:00Z
pubs.issue	21
pubs.publication-status	Published
pubs.volume	13
utslib.citation.issue	21

Abstract:

Facilitating the charge separation of semiconductor photocatalysts to increase the photocatalytic CO₂ reduction activity has become a great challenge for sustainable energy conversion. Herein, the surface halogen-modified defect-rich Bi₂ WO₆ nanosheets have been successfully prepared to address the aforementioned challenge. Importantly, the modification of surface with halogen atoms is beneficial for the adsorption and activation for CO₂ molecules and charge separation. These properties have been analyzed by experimental and theoretical methods. DFT calculations revealed that the modification of the Bi₂ WO₆ surface with Br atoms can decrease the formation energy of the *COOH intermediate, which accelerates CO₂ conversion. All halogen-modified defect-rich Bi₂ WO₆ nanosheets showed an enhanced photocatalytic CO₂ reduction activity. Specifically, Br-Bi₂ WO₆ exhibited the best CO generation rate of 13.8 μmol g^-1 h^-1 , which is roughly 7.3 times as high as the unmodified defect-rich Bi₂ WO₆ (1.9 μmol g^-1 h^-1 ). Moreover, in the presence of a cocatalyst (cobalt phthalocyanine) and a sacrificial agent (triethanolamine), Br-Bi₂ WO₆ exhibited an even further improved CO generation rate of 187 μmol g^-1 h^-1 . This finding provides a new approach to optimize the CO₂ reduction pathway of semiconductor photocatalysts, which is beneficial to develop highly efficient CO₂ reduction photocatalysts.

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