通过有效电子传递改善磺胺嘧啶光降解的新型氢键有机框架/g-C3N4 异质结

IF 4.1 3区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2024-08-12 DOI:10.1016/j.jphotochem.2024.115946
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摘要

作为最广泛使用的抗生素之一,磺胺甲噁唑(SDZ)会对水生生物造成危害,并加速耐抗生素细菌的进化,从而对生态环境造成重大健康风险。金属卟啉氢键有机框架(PFC-72)具有高比表面积、宽采光范围、稳定的物理化学性质和半导体特性,在光催化领域具有广阔的应用前景。在此,我们采用一步溶剂热法构建了一种高效光催化剂 PFC-72/g-C3N4,用于光催化降解 SDZ。当PFC-72的掺杂量为10%时,在可见光照射120 min后,SDZ的光催化降解效率可达96.82%,且PFC-72/g-C3N4表现出优异的结构稳定性。通过增加比表面积、提高可见光的吸收范围以及抑制光生电子-空穴对的重组,SDZ 的光催化效率得以提高。此外,还通过 UPLC-MS/MS 分析确定了 SDZ 在 PFC-72/g-C3N4 中的光降解途径。最后,通过自由基掩蔽实验检测了体系中的主要活性物种(-O2-、hVB+ 和 -OH),并阐明了光催化机理。这项工作研究了一种新型高效的基于卟啉-HOF 的光催化剂,它在降解 SDZ 方面具有很大的潜力。
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A novel hydrogen-bonded organic framework/g-C3N4 heterojunction for improved sulfadiazine photodegradation via effective electron transfer

As one of the most widely used antibiotics, sulfamethoxazole (SDZ) poses significant health risks to the ecological environment by causing harm to aquatic organisms and accelerating evolution of antibiotic resistant bacteria. Metalloporphyrin hydrogen-bonded organic framework (PFC-72) demonstrates promising prospect in the field of photocatalysis owing to its high specific surface area, wide light harvesting range, stable physical and chemical properties, and semiconductor properties. Herein, we constructed an efficient photocatalyst PFC-72/g-C3N4 by one-step solvent thermal method for photocatalytic degradation of SDZ. When doping content of PFC-72 is 10 %, photocatalytic degradation efficiency of SDZ can reach 96.82 % after 120 min of visible light irradiation, and PFC-72/g-C3N4 exhibits excellent structural stability. The photocatalytic efficiency of SDZ is improved by increasing specific surface area, enhancing absorption range of visible light, and inhibiting recombination of photogenerated electron-hole pairs. In addition, photodegradation pathways of SDZ in PFC-72/g-C3N4 was determined by UPLC-MS/MS analysis. Finally, dominant reactive species (·O2, hVB+, and ·OH) in the system were detected through free radical masking experiments, and photocatalytic mechanism was clarified. This work investigates a novel and efficient porphyrin-HOF based photocatalyst, which has great potential for degradation of SDZ.

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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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