Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion

Photocatalysis is an emerging alternative to convert CO2 into relevant products, but it faces technological challenges related to charge recombination and low efficiency. Thermally coupled gas phase photocatalysis can address these issues by lowering reaction temperatures and improving process effic...

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Main Authors: S. Vaquero-Vílchez, P. Nimax, E. Valtierra-Martinez, I. Ayesta, I. Agirrezabal-Telleria
Format: Article
Language:English
Published: Elsevier 2025-05-01
Series:Journal of CO2 Utilization
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Online Access:http://www.sciencedirect.com/science/article/pii/S2212982025000526
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author S. Vaquero-Vílchez
P. Nimax
E. Valtierra-Martinez
I. Ayesta
I. Agirrezabal-Telleria
author_facet S. Vaquero-Vílchez
P. Nimax
E. Valtierra-Martinez
I. Ayesta
I. Agirrezabal-Telleria
author_sort S. Vaquero-Vílchez
collection DOAJ
description Photocatalysis is an emerging alternative to convert CO2 into relevant products, but it faces technological challenges related to charge recombination and low efficiency. Thermally coupled gas phase photocatalysis can address these issues by lowering reaction temperatures and improving process efficiency. This work demonstrates that defect engineering, combined with Pt impregnation at various metal dispersion and sizes, can enhance photocatalytic properties in g-C3N4 materials. Structural changes in g-C3N4 and Pt oxidation state modification, significantly impact CO productivity from CO2. This study investigates how thermal treatments in H2 affect defect and thus vacancy formation in g-C3N4. Materials with 2 wt% Pt2+ species generate C–N3 vacancies, while Pt0 species with the same content lead to both C–N3 and N–C3 vacancies– within g-C3N4. These differences exhibit distinct reaction trends under dark conditions or upon light irradiation. To further understand these effects, detailed XPS analyses clarify the impact of reaction conditions on the material after pretreatment and catalysis. The findings show that g-C3N4 materials can reform their C–Nbonds after electron excitation through light exposure, enhancing and stabilizing the reaction's productivity. As a result, CO productivities up to 1.1 mmol·gcat−1·h−1 are achieved. This work is expected to contribute to understanding the effect of thermal treatment on carbon nitrides, particularly regarding defect engineering, and more broadly, the effects of temperature in photocatalysis.
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spelling doaj-art-cf9b0a3eb217433c8aff86f43591fb992025-08-20T02:18:55ZengElsevierJournal of CO2 Utilization2212-98392025-05-019510306810.1016/j.jcou.2025.103068Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversionS. Vaquero-Vílchez0P. Nimax1E. Valtierra-Martinez2I. Ayesta3I. Agirrezabal-Telleria4Department of Chemical and Environmental Engineering, Engineering School of Bilbao, University of the Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, Bilbao 48013, Spain; Corresponding author.Department of Chemical and Environmental Engineering, Engineering School of Bilbao, University of the Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, Bilbao 48013, SpainDepartment of Chemical and Environmental Engineering, Engineering School of Bilbao, University of the Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, Bilbao 48013, SpainDepartment of Applied Mathematics, Engineering School of Bilbao, University of the Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, Bilbao 48013, SpainDepartment of Chemical and Environmental Engineering, Engineering School of Bilbao, University of the Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, Bilbao 48013, SpainPhotocatalysis is an emerging alternative to convert CO2 into relevant products, but it faces technological challenges related to charge recombination and low efficiency. Thermally coupled gas phase photocatalysis can address these issues by lowering reaction temperatures and improving process efficiency. This work demonstrates that defect engineering, combined with Pt impregnation at various metal dispersion and sizes, can enhance photocatalytic properties in g-C3N4 materials. Structural changes in g-C3N4 and Pt oxidation state modification, significantly impact CO productivity from CO2. This study investigates how thermal treatments in H2 affect defect and thus vacancy formation in g-C3N4. Materials with 2 wt% Pt2+ species generate C–N3 vacancies, while Pt0 species with the same content lead to both C–N3 and N–C3 vacancies– within g-C3N4. These differences exhibit distinct reaction trends under dark conditions or upon light irradiation. To further understand these effects, detailed XPS analyses clarify the impact of reaction conditions on the material after pretreatment and catalysis. The findings show that g-C3N4 materials can reform their C–Nbonds after electron excitation through light exposure, enhancing and stabilizing the reaction's productivity. As a result, CO productivities up to 1.1 mmol·gcat−1·h−1 are achieved. This work is expected to contribute to understanding the effect of thermal treatment on carbon nitrides, particularly regarding defect engineering, and more broadly, the effects of temperature in photocatalysis.http://www.sciencedirect.com/science/article/pii/S2212982025000526Gas phase CO2 photoreductionCarbon nitrideDefect engineeringVacanciesPhotocatalysis
spellingShingle S. Vaquero-Vílchez
P. Nimax
E. Valtierra-Martinez
I. Ayesta
I. Agirrezabal-Telleria
Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion
Journal of CO2 Utilization
Gas phase CO2 photoreduction
Carbon nitride
Defect engineering
Vacancies
Photocatalysis
title Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion
title_full Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion
title_fullStr Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion
title_full_unstemmed Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion
title_short Photocatalytic and surface consequences of thermal treatments on Pt nanoparticles onto carbon nitrides during CO2-to-CO conversion
title_sort photocatalytic and surface consequences of thermal treatments on pt nanoparticles onto carbon nitrides during co2 to co conversion
topic Gas phase CO2 photoreduction
Carbon nitride
Defect engineering
Vacancies
Photocatalysis
url http://www.sciencedirect.com/science/article/pii/S2212982025000526
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