Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis
Graphitic carbon nitride (C3N4) is a promising photocatalyst due to its suitable band gap and polymer properties, but its efficiency is limited by the poor separation of photoinduced electron/hole (e–/h+) pairs. To address this issue, we propose creating N vacancies within the layers and bridging K...
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Elsevier
2025-05-01
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| Series: | Journal of Materiomics |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2352847824002089 |
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| author | Xiao Xu Yao Xiao Xuelian Xu Sónia A.C. Carabineiro Junjiang Zhu |
| author_facet | Xiao Xu Yao Xiao Xuelian Xu Sónia A.C. Carabineiro Junjiang Zhu |
| author_sort | Xiao Xu |
| collection | DOAJ |
| description | Graphitic carbon nitride (C3N4) is a promising photocatalyst due to its suitable band gap and polymer properties, but its efficiency is limited by the poor separation of photoinduced electron/hole (e–/h+) pairs. To address this issue, we propose creating N vacancies within the layers and bridging K single-atoms between the C3N4 layers through the self-assembly of potassium citrate and melamine–urea monomers. The introduction of N vacancies disrupts the symmetry of C3N4, promoting electron transfer along the delocalized π-conjugated network, while the presence of K atoms provides channels for electron transfer between the layers by forming NKN bridges, thereby leading to significant enhancement in the separation and transfer of e–/h+ pairs across spatial dimension. As expected, the co-modified C3N4, with N vacancies and K single-atoms (designated as CN-K-VN), exhibits excellent photocatalytic performance, with reaction rate constant of 9.69 × 10−2 min−1 (7.39 × 10−2 min−1 in real water environment) for tetracycline, achieving 80% degradation of tetracycline within 20 min. The reaction mechanism, as well as the toxicity of the degradation intermediates, is deeply discussed. This study provides a strategy to enhance the spatial separation of electrons for photocatalyst, highlighting its significance role in photocatalysis. |
| format | Article |
| id | doaj-art-cb90ea699f784ea993774d76b692e2a8 |
| institution | DOAJ |
| issn | 2352-8478 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Journal of Materiomics |
| spelling | doaj-art-cb90ea699f784ea993774d76b692e2a82025-08-20T03:15:17ZengElsevierJournal of Materiomics2352-84782025-05-0111310096910.1016/j.jmat.2024.100969Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysisXiao Xu0Yao Xiao1Xuelian Xu2Sónia A.C. Carabineiro3Junjiang Zhu4Hubei Key Laboratory of Biomass Fibers and Eco-dyeing & Finishing, School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200, ChinaHubei Key Laboratory of Biomass Fibers and Eco-dyeing & Finishing, School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200, ChinaHubei Key Laboratory of Biomass Fibers and Eco-dyeing & Finishing, School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200, ChinaLAQV-REQUIMTE, Department of Chemistry, NOVA School of Science and Technology, Universidade NOVA de Lisboa, Largo da Torre, 2829-516, Caparica, PortugalHubei Key Laboratory of Biomass Fibers and Eco-dyeing & Finishing, School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200, China; Corresponding author.Graphitic carbon nitride (C3N4) is a promising photocatalyst due to its suitable band gap and polymer properties, but its efficiency is limited by the poor separation of photoinduced electron/hole (e–/h+) pairs. To address this issue, we propose creating N vacancies within the layers and bridging K single-atoms between the C3N4 layers through the self-assembly of potassium citrate and melamine–urea monomers. The introduction of N vacancies disrupts the symmetry of C3N4, promoting electron transfer along the delocalized π-conjugated network, while the presence of K atoms provides channels for electron transfer between the layers by forming NKN bridges, thereby leading to significant enhancement in the separation and transfer of e–/h+ pairs across spatial dimension. As expected, the co-modified C3N4, with N vacancies and K single-atoms (designated as CN-K-VN), exhibits excellent photocatalytic performance, with reaction rate constant of 9.69 × 10−2 min−1 (7.39 × 10−2 min−1 in real water environment) for tetracycline, achieving 80% degradation of tetracycline within 20 min. The reaction mechanism, as well as the toxicity of the degradation intermediates, is deeply discussed. This study provides a strategy to enhance the spatial separation of electrons for photocatalyst, highlighting its significance role in photocatalysis.http://www.sciencedirect.com/science/article/pii/S2352847824002089C3N4N vacanciesK single-atomSpatial separation of electronsPhotocatalysis |
| spellingShingle | Xiao Xu Yao Xiao Xuelian Xu Sónia A.C. Carabineiro Junjiang Zhu Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis Journal of Materiomics C3N4 N vacancies K single-atom Spatial separation of electrons Photocatalysis |
| title | Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis |
| title_full | Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis |
| title_fullStr | Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis |
| title_full_unstemmed | Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis |
| title_short | Dual-site engineering of N vacancies and K single-atoms in C3N4: Enabling spatial charge transfer channels for photocatalysis |
| title_sort | dual site engineering of n vacancies and k single atoms in c3n4 enabling spatial charge transfer channels for photocatalysis |
| topic | C3N4 N vacancies K single-atom Spatial separation of electrons Photocatalysis |
| url | http://www.sciencedirect.com/science/article/pii/S2352847824002089 |
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