Three-Phase Interface Construction on Hydrophobic Carbonaceous Catalysts for Highly Active and Selective Photocatalytic CO<inf>2</inf> Conversion

Huang, QS; Chu, C; Li, Q; Liu, Q; Liu, X; Sun, J; Ni, BJ; Mao, S

Three-Phase Interface Construction on Hydrophobic Carbonaceous Catalysts for Highly Active and Selective Photocatalytic CO<inf>2</inf> Conversion

Huang, QS Chu, C Li, Q Liu, Q Liu, X Sun, J Ni, BJ Mao, S

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Publisher:: AMER CHEMICAL SOC
Publication Type:: Journal Article
Citation:: ACS Catalysis, 2023, 13, (17), pp. 11232-11243
Issue Date:: 2023-09-01

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Field	Value	Language
dc.contributor.author	Huang, QS
dc.contributor.author	Chu, C
dc.contributor.author	Li, Q
dc.contributor.author	Liu, Q
dc.contributor.author	Liu, X
dc.contributor.author	Sun, J
dc.contributor.author	Ni, BJ
dc.contributor.author	Mao, S
dc.date.accessioned	2024-04-12T09:02:38Z
dc.date.available	2024-04-12T09:02:38Z
dc.date.issued	2023-09-01
dc.identifier.citation	ACS Catalysis, 2023, 13, (17), pp. 11232-11243
dc.identifier.issn	2155-5435
dc.identifier.issn	2155-5435
dc.identifier.uri	http://hdl.handle.net/10453/177852
dc.description.abstract	The ever-increasing concern for adverse climate change has stimulated great research enthusiasm for CO2 conversion. The photocatalytic CO2 reduction reaction (CO2RR) has become one of the promising approaches to converting CO2 into value-added fuels. However, CO2RR suffers from intense competition from the hydrogen evolution reaction (HER) for electrons in aqueous solution due to the limited mass transfer of CO2 in water. In this study, we propose to construct the three-phase interface on the photocatalyst surface by decorating with a hydrophobic carbonaceous cocatalyst to achieve efficient contact of CO2 (gas), catalyst (solid), and water (liquid). The decorated photocatalyst exhibits significantly improved CO2-to-CH4 activity, and the CO2RR selectivity is greatly elevated from 61 to 97%. It is demonstrated that the hydrophobic cocatalyst plays a critical role in regulating the CO2RR performance by increasing the interfacial CO2 concentration. Molecular dynamics simulations further reveal that the hydrophobic microenvironment is constructed by preventing the hydrogen bond formation on the carbonaceous cocatalyst surface. Overall, this study provides a general method to relieve the CO2 mass transfer limit to accelerate the CO2RR in water.
dc.language	English
dc.publisher	AMER CHEMICAL SOC
dc.relation.ispartof	ACS Catalysis
dc.relation.isbasedon	10.1021/acscatal.3c01612
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	0302 Inorganic Chemistry, 0305 Organic Chemistry, 0904 Chemical Engineering
dc.subject.classification	3106 Industrial biotechnology
dc.subject.classification	3405 Organic chemistry
dc.subject.classification	3406 Physical chemistry
dc.title	Three-Phase Interface Construction on Hydrophobic Carbonaceous Catalysts for Highly Active and Selective Photocatalytic CO<inf>2</inf> Conversion
dc.type	Journal Article
utslib.citation.volume	13
utslib.for	0302 Inorganic Chemistry
utslib.for	0305 Organic Chemistry
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
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	2024-04-12T09:02:33Z
pubs.issue	17
pubs.publication-status	Published
pubs.volume	13
utslib.citation.issue	17

Abstract:

The ever-increasing concern for adverse climate change has stimulated great research enthusiasm for CO2 conversion. The photocatalytic CO2 reduction reaction (CO2RR) has become one of the promising approaches to converting CO2 into value-added fuels. However, CO2RR suffers from intense competition from the hydrogen evolution reaction (HER) for electrons in aqueous solution due to the limited mass transfer of CO2 in water. In this study, we propose to construct the three-phase interface on the photocatalyst surface by decorating with a hydrophobic carbonaceous cocatalyst to achieve efficient contact of CO2 (gas), catalyst (solid), and water (liquid). The decorated photocatalyst exhibits significantly improved CO2-to-CH4 activity, and the CO2RR selectivity is greatly elevated from 61 to 97%. It is demonstrated that the hydrophobic cocatalyst plays a critical role in regulating the CO2RR performance by increasing the interfacial CO2 concentration. Molecular dynamics simulations further reveal that the hydrophobic microenvironment is constructed by preventing the hydrogen bond formation on the carbonaceous cocatalyst surface. Overall, this study provides a general method to relieve the CO2 mass transfer limit to accelerate the CO2RR in water.

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http://hdl.handle.net/10453/177852