Efficient Photocatalytic Desulfurization in Air through Improved Photogenerated Carriers Separation in MOF MIL101/Carbon Dots-g-C3N4 Nanocomposites.

Zhou, X; Wang, T; He, D; Chen, P; Liu, H; Lv, H; Wu, H; Su, D; Pang, H; Wang, C

Efficient Photocatalytic Desulfurization in Air through Improved Photogenerated Carriers Separation in MOF MIL101/Carbon Dots-g-C3N4 Nanocomposites.

Zhou, X Wang, T He, D Chen, P Liu, H Lv, H Wu, H Su, D

Pang, H Wang, C

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Publisher:: WILEY-V C H VERLAG GMBH
Publication Type:: Journal Article
Citation:: Angew Chem Int Ed Engl, 2024, 63, (35), pp. e202408989
Issue Date:: 2024-08-26

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Field	Value	Language
dc.contributor.author	Zhou, X
dc.contributor.author	Wang, T
dc.contributor.author	He, D
dc.contributor.author	Chen, P
dc.contributor.author	Liu, H
dc.contributor.author	Lv, H
dc.contributor.author	Wu, H
dc.contributor.author	Su, D https://orcid.org/0000-0002-3972-8205
dc.contributor.author	Pang, H
dc.contributor.author	Wang, C
dc.date.accessioned	2025-01-02T23:47:17Z
dc.date.available	2025-01-02T23:47:17Z
dc.date.issued	2024-08-26
dc.identifier.citation	Angew Chem Int Ed Engl, 2024, 63, (35), pp. e202408989
dc.identifier.issn	1433-7851
dc.identifier.issn	1521-3773
dc.identifier.uri	http://hdl.handle.net/10453/182869
dc.description.abstract	The extensive industrial applications of fuel oil, a critical strategic resource, are accompanied by significant environmental and health concerns due to the presence of sulfur-containing compounds in its composition, which result in hazardous combustion waste. Extensive research has been conducted to develop technologies for low-vulcanization fuel production to address this issue. Consequently, the investigation of catalysts for environmentally friendly and safe photocatalytic desulfurization becomes imperative. To that end, we have designed efficient MIL-101(Fe)/CQDs@g-C3N4 (MIL101/CDs-C3N4) Z-scheme heterojunction photocatalysts with high carrier separation and mobility through a thermal polymerization-hydrothermal strategy. The high concentration of photogenerated carriers facilitates the activation of oxygen and H2O2, leading to increased production of ROS (⋅O2 -, ⋅OH, h+), thereby enhancing the photocatalytic desulfurization (PODS). Additionally, DFT (Density functional theory) calculations were utilized to determine the electron migration pathways of the catalysts and adsorption energies of DBT (dibenzothiophene). Moreover, Gibbs free energy calculations indicated that MIL101/CDs-C3N4 exhibited the lowest activation energy for oxygen and H2O2. The mechanism of photocatalytic desulfurization was proposed through a combination of theoretical calculations and experimental studies. This study provides guidance for the development of MOF-based Z-scheme systems and their practical application in desulfurization processes.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	WILEY-V C H VERLAG GMBH
dc.relation.ispartof	Angew Chem Int Ed Engl
dc.relation.isbasedon	10.1002/anie.202408989
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	03 Chemical Sciences
dc.subject.classification	Organic Chemistry
dc.subject.classification	34 Chemical sciences
dc.title	Efficient Photocatalytic Desulfurization in Air through Improved Photogenerated Carriers Separation in MOF MIL101/Carbon Dots-g-C3N4 Nanocomposites.
dc.type	Journal Article
utslib.citation.volume	63
utslib.location.activity	Germany
utslib.for	03 Chemical Sciences
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
utslib.copyright.status	closed_access	*
dc.date.updated	2025-01-02T23:47:15Z
pubs.issue	35
pubs.publication-status	Published
pubs.volume	63
utslib.citation.issue	35

Abstract:

The extensive industrial applications of fuel oil, a critical strategic resource, are accompanied by significant environmental and health concerns due to the presence of sulfur-containing compounds in its composition, which result in hazardous combustion waste. Extensive research has been conducted to develop technologies for low-vulcanization fuel production to address this issue. Consequently, the investigation of catalysts for environmentally friendly and safe photocatalytic desulfurization becomes imperative. To that end, we have designed efficient MIL-101(Fe)/CQDs@g-C3N4 (MIL101/CDs-C3N4) Z-scheme heterojunction photocatalysts with high carrier separation and mobility through a thermal polymerization-hydrothermal strategy. The high concentration of photogenerated carriers facilitates the activation of oxygen and H2O2, leading to increased production of ROS (⋅O2 -, ⋅OH, h+), thereby enhancing the photocatalytic desulfurization (PODS). Additionally, DFT (Density functional theory) calculations were utilized to determine the electron migration pathways of the catalysts and adsorption energies of DBT (dibenzothiophene). Moreover, Gibbs free energy calculations indicated that MIL101/CDs-C3N4 exhibited the lowest activation energy for oxygen and H2O2. The mechanism of photocatalytic desulfurization was proposed through a combination of theoretical calculations and experimental studies. This study provides guidance for the development of MOF-based Z-scheme systems and their practical application in desulfurization processes.

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http://hdl.handle.net/10453/182869