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Dual-site engineering of N vacancies and K single-atoms in C3N4
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Resumo(s)
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 N[sbnd]K[sbnd]N 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.
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Funding Information:
This work was financially supported by the National Natural Science Foundation of China (42277485, 21976141), the Department of Science and Technology of Hubei Province (2021CFA034), the Knowledge Innovation Program of Wuhan–Shuguang Project (No. 2023020201020369). SACC acknowledges FCT/MCTES (Fundação para a Ciência e Tecnologia and Ministério da Ciência, Tecnologia e Ensino Superior) for project DOIs: 10.54499/LA/P/0008/2020, 10.54499/UIDP/50006/2020, 10.54499/UIDB/50006/2020 from LAQV and for the Scientific Employment Stimulus - Institutional Call (DOI 10.54499/CEECINST/00102/2018/CP1567/CT0026). We thank the Analytical and Testing Center of Wuhan Textile University for LC-MS test.
Publisher Copyright:
© 2024 The Authors
Palavras-chave
C3N4 K single-atom N vacancies Photocatalysis Spatial separation of electrons Electronic, Optical and Magnetic Materials Surfaces, Coatings and Films Metals and Alloys