Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in porous carbon nitride

Yang Ding; Soumyajit Maitra; Daniel Arenas Esteban; Sara Bals; Henk Vrielinck; Tarek Barakat; Subhasis Roy; Gustaaf Van Tendeloo; Jing Liu; Yu Li; Alexandru Vlad; Bao Lian Su

doi:10.1016/j.xcrp.2022.100874

Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in porous carbon nitride

Yang Ding, Soumyajit Maitra, Daniel Arenas Esteban, Sara Bals, Henk Vrielinck, Tarek Barakat, Subhasis Roy, Gustaaf Van Tendeloo, Jing Liu, Yu Li, Alexandru Vlad, Bao Lian Su

Universite de Namur

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

Résumé

Artificial photosynthesis of H₂O₂, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H₂O₂ artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C₃N₄ through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (^⋅O₂⁻) formation, significantly boosting the H₂O₂ photocatalytic production. The developed photocatalyst shows an H₂O₂ evolution rate of 6287.5 μM g⁻¹ h⁻¹ under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C₃N₄-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H₂O₂ production.

langue originale	Anglais
Numéro d'article	100874
journal	Cell Reports Physical Science
Volume	3
Numéro de publication	5
Les DOIs	https://doi.org/10.1016/j.xcrp.2022.100874
Etat de la publication	Publié - 18 mai 2022

Financement

Y.D. thanks the China Scholarship Council (201808310127) for financial support. This work is financially supported by the National Natural Science Foundation of China (U1663225), Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R52) of the Chinese Ministry of Education, Program of Introducing Talents of Discipline to Universities-Plan 111 (grant no. B20002) from the Ministry of Science and Technology and the Ministry of Education of China, and the National Key R&D Program of China (2016YFA0202602). This research was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project “DepollutAir”. Y.D. carried out all experiments and wrote the paper, and T.B. helped the realization of the experiments. S.M. and S.R. conducted the DFT calculations. D.A.E. S.B. and G.V.T conducted the HAADF-TEM and iDPC-STEM characterizations. H.V. carried out the EPR analysis. J.L, A.V. and Y.L. took part in the establishment of research project. All the authors discussed the results and verified and revised the paper. Y.L. helped to finalize the manuscript. B.-L.S. established the research direction, conceived the project, provided the scientific guidance and project realization ideas, and revised and finalized the paper. The authors declare no competing interests. Y.D. thanks the China Scholarship Council ( 201808310127 ) for financial support. This work is financially supported by the National Natural Science Foundation of China ( U1663225 ), Program for Changjiang Scholars and Innovative Research Team in University ( IRT_15R52 ) of the Chinese Ministry of Education , Program of Introducing Talents of Discipline to Universities-Plan 111 (grant no. B20002 ) from the Ministry of Science and Technology and the Ministry of Education of China , and the National Key R&D Program of China ( 2016YFA0202602 ). This research was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project “DepollutAir”.

Bailleurs de fonds	Numéro du bailleur de fonds
Chinese Ministry of Education, the Program of Introducing Talents of Discipline to Universities-Plan 111	B20002
Chinese Ministry of Education, the Program of Introducing Talents of Discipline to Universities-Plan 111
European Commission Interreg
National Natural Science Foundation of China	U1663225
National Natural Science Foundation of China
Ministry of Education of the People's Republic of China
Ministry of Science and Technology of the People's Republic of China
China Scholarship Council	201808310127
China Scholarship Council
National Key Research and Development Program of China	2016YFA0202602
National Key Research and Development Program of China
Program for Changjiang Scholars and Innovative Research Team in University	IRT_15R52
Program for Changjiang Scholars and Innovative Research Team in University

SDG des Nations Unies

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title = "Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in porous carbon nitride",

abstract = "Artificial photosynthesis of H2O2, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H2O2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C3N4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (⋅O2−) formation, significantly boosting the H2O2 photocatalytic production. The developed photocatalyst shows an H2O2 evolution rate of 6287.5 μM g−1 h−1 under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C3N4-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H2O2 production.",

keywords = "artificial photosynthesis, carbon vacancies, freeze-drying, HO production, hierarchical porous carbon nitride",

author = "Yang Ding and Soumyajit Maitra and Esteban, {Daniel Arenas} and Sara Bals and Henk Vrielinck and Tarek Barakat and Subhasis Roy and {Van Tendeloo}, Gustaaf and Jing Liu and Yu Li and Alexandru Vlad and Su, {Bao Lian}",

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AU - Ding, Yang

AU - Maitra, Soumyajit

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AU - Bals, Sara

AU - Vrielinck, Henk

AU - Barakat, Tarek

AU - Roy, Subhasis

AU - Van Tendeloo, Gustaaf

AU - Liu, Jing

AU - Li, Yu

AU - Vlad, Alexandru

AU - Su, Bao Lian

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N2 - Artificial photosynthesis of H2O2, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H2O2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C3N4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (⋅O2−) formation, significantly boosting the H2O2 photocatalytic production. The developed photocatalyst shows an H2O2 evolution rate of 6287.5 μM g−1 h−1 under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C3N4-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H2O2 production.

AB - Artificial photosynthesis of H2O2, an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H2O2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C3N4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical (⋅O2−) formation, significantly boosting the H2O2 photocatalytic production. The developed photocatalyst shows an H2O2 evolution rate of 6287.5 μM g−1 h−1 under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C3N4-based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H2O2 production.

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Photochemical production of hydrogen peroxide by digging pro-superoxide radical carbon vacancies in porous carbon nitride

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SDG des Nations Unies

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Physico-chimie et caractérisation (PC2)

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