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具有氧空位(Ov)的s型3D/3D Bi/BiOBr/P掺杂g-C3N4用于药物光降解:原位产生羟基自由基及等离子体诱导稳定性

s-scheme3D/3D Bi/BiOBr/P Doped g-C3 N4 with Oxygen Vacancies (Ov) for Photodegradation of Pharmaceuticals: In-situ HO Production and Plasmon Induced Stability.

作者信息

Malefane Mope E, Managa Muthumuni, Nkambule Thabo T I, Kuvarega Alex T

机构信息

Institute for Nanotechnology and Water Sustainability, College of Science, Engineering and Technology, University of South Africa, Florida, Johannesburg, 1709, South Africa.

出版信息

ChemSusChem. 2025 Jan 14;18(2):e202401471. doi: 10.1002/cssc.202401471. Epub 2024 Oct 18.

Abstract

Complications accompanying photocatalyst stability and recombination of exciton charges in pollutants degradation has been addressed through the construction of heterojunctions, especially S-scheme heterojunction with strong and distinctive redox centres. Herein, an S-scheme BiOBr (BOR) and g-CNPO (CNPO) catalyst (BORCNPO) with oxygen vacancy (Ov) was synthesized for levofloxacin (LVX) and oxytetracycline (OTC) photodegradation under visible light. The 3D/3D BORCNPO catalyst possessed C-O-Br bridging bonds for efficient charge transfer during the fabrication of S-scheme heterojunction. In-situ HO formation affirmed by potassium titanium (IV) oxalate spectrophotometric method improved the mineralization ability of BORCNPO7.5 catalyst. Bi surface plasmon resonance (SPR) enhanced formation and involvement of ⋅O and the stability of the catalyst which increased reaction rate with increasing cycling experiments. XPS and radical trapping experiments supported the S-scheme charge transfer mechanism formation with high degradation rate of LVX which was 3 times higher than OTC degradation rate. Mineralization of pollutants and their intermediates were demonstrated with florescence excitation and emission matrix (FEEM) and quadruple time of flight high performance liquid chromatography (QTOF-HPLC). This work advances development of highly stable and efficient catalysts for photodegradation of pollutants through the formation of S-scheme heterostructure.

摘要

通过构建异质结,特别是具有强且独特氧化还原中心的S型异质结,解决了光催化剂稳定性和激子电荷在污染物降解中复合的问题。在此,合成了一种具有氧空位(Ov)的S型BiOBr(BOR)和g-CNPO(CNPO)催化剂(BORCNPO),用于在可见光下光降解左氧氟沙星(LVX)和土霉素(OTC)。3D/3D BORCNPO催化剂在构建S型异质结过程中具有C-O-Br桥键,可实现高效电荷转移。通过草酸钛(IV)钾分光光度法证实的原位羟基自由基(HO)形成提高了BORCNPO7.5催化剂的矿化能力。Bi表面等离子体共振(SPR)增强了超氧阴离子自由基(⋅O )的形成和参与以及催化剂的稳定性,随着循环实验次数增加,反应速率提高。X射线光电子能谱(XPS)和自由基捕获实验支持了S型电荷转移机制的形成,LVX的高降解率是OTC降解率的3倍。通过荧光激发发射矩阵(FEEM)和四极杆飞行时间高效液相色谱(QTOF-HPLC)证明了污染物及其中间体的矿化。这项工作通过形成S型异质结构推动了用于光降解污染物的高稳定性和高效催化剂的开发。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/726a/11739848/e7106d24c939/CSSC-18-e202401471-g006.jpg

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