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TiO2 包覆的 PET 光催化剂在可见光下对合成废水和实际废水中活性黑 5 的光催化降解

Photocatalytic degradation of reactive black 5 from synthetic and real wastewater under visible light with TiO coated PET photocatalysts.

作者信息

Mohammadi-Galangash Mohsen, Mousavi Seyedeh-Khadijeh, Shirzad-Siboni Mehdi

机构信息

Department of Environmental Sciences and Engineering, Faculty of Natural Resources, University of Guilan, Sowmeh Sara, Guilan,, Iran.

Research Center of Health and Environment, Guilan University of Medical Sciences, Rasht, Iran.

出版信息

Sci Rep. 2025 Apr 24;15(1):14314. doi: 10.1038/s41598-025-95091-x.

DOI:10.1038/s41598-025-95091-x
PMID:40274880
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12022298/
Abstract

The photocatalytic removal of Reactive Black 5 (RB5) was investigated using a titanium dioxide-polyethylene terephthalate (TiO-PET) catalyst under visible (VIS) light. The sol-gel method was employed for the fabrication of the TiO-coated PET catalyst, which was then characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and elemental mapping (MAP) analysis. This study examined the reaction kinetics using the one-factor-at-a-time (OFAT) approach and evaluates the effects of various parameters, including pH (3-11), catalyst dosage (0.1-1 g L), contact time (15-120 min), RB5 concentration (10-50 mg L), hydrogen peroxide (HO) content (2-100 mM), purging gases, organic compound types, and ionic strength, on the photocatalytic removal of RB5. Under optimal conditions (pH= 3, [RB5]= 20 mg L, nanocatalyst dosage= 0.5 g L), 99.99% of the dye was removed after 120 min. Increasing the RB5 concentration (10-50 mg L) resulted in a decrease in the observed reaction rate constant (k) from 0.052 to 0.0017 min, while the calculated electrical energy per order (EEO) increased from 11.08 to 338.82 kWh m. Furthermore, the total operating cost of the light emitting diode (LED)/TiO-PET process (3 USD kg) was lower than that of other photocatalytic processes, including LED/TiO (4.73 USD kg), LED/PET (40 USD kg), and LED (63.16 USD kg). The removal of RB5 was negatively affected by the presence of HO, O and N gases, organic compounds, and ionic species. Radical quenching experiments confirmed that hydroxyl radicals (OH) were the dominant reactive species responsible for RB5 degradation. The RB5 removal efficiency using the LED/TiO-PET method (99.99%) was significantly higher than that of the LED/TiO method (63.42%). Desorption experiments demonstrated excellent catalyst stability, maintaining catalytic activity for up to five sequential cycles. GC-MS analysis identified several intermediate degradation products, including 1,2-benzenedicarboxylic acid, benzoic acid (2-amino-, methyl ester), benzene [(methylsulfonyl) methyl], phenol, 4-naphthalenedione, acetic acid, and propionic acid. Moreover, the removal efficiency in drinking water samples was approximately 63.31%, whereas for real textile wastewater samples, it reached 96.66%. Toxicity tests conducted on the final treated solutions confirmed no toxicity toward Daphnia magna, demonstrating the effectiveness of the LED/TiO-PET method in degrading both RB5 dye and its toxic by-products.

摘要

采用二氧化钛-聚对苯二甲酸乙二酯(TiO-PET)催化剂在可见光(VIS)下研究了活性黑5(RB5)的光催化去除。采用溶胶-凝胶法制备TiO包覆的PET催化剂,然后用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描电子显微镜(SEM)、能量色散X射线光谱(EDX)和元素映射(MAP)分析对其进行表征。本研究采用一次单因素(OFAT)方法研究反应动力学,并评估了各种参数对RB5光催化去除的影响,这些参数包括pH值(3-11)、催化剂用量(0.1-1 g/L)、接触时间(15-120分钟)、RB5浓度(10-50 mg/L)、过氧化氢(H₂O₂)含量(2-100 mM)、吹扫气体、有机化合物类型和离子强度。在最佳条件下(pH = 3,[RB5] = 20 mg/L,纳米催化剂用量 = 0.5 g/L),120分钟后99.99%的染料被去除。RB5浓度从10 mg/L增加到50 mg/L导致观察到的反应速率常数(k)从0.052降至0.0017 min⁻¹,而计算得出的每级电能(EEO)从11.08增加到338.82 kWh/m³。此外,发光二极管(LED)/TiO-PET工艺的总运行成本(3美元/kg)低于其他光催化工艺,包括LED/TiO(4.73美元/kg)、LED/PET(40美元/kg)和LED(63.16美元/kg)。H₂O₂、O₂和N₂气体、有机化合物和离子物种的存在对RB5的去除产生负面影响。自由基猝灭实验证实羟基自由基(·OH)是负责RB5降解的主要活性物种。LED/TiO-PET法对RB5的去除效率(99.99%)显著高于LED/TiO法(63.42%)。解吸实验表明催化剂具有优异的稳定性,在连续五个循环中均保持催化活性。气相色谱-质谱(GC-MS)分析确定了几种中间降解产物,包括1,2-苯二甲酸、苯甲酸(2-氨基-,甲酯)、苯[(甲基磺酰基)甲基]、苯酚、4-萘二酮、乙酸和丙酸。此外,饮用水样品中的去除效率约为63.31%,而对于实际纺织废水样品,去除效率达到96.66%。对最终处理溶液进行的毒性测试证实对大型溞无毒性,证明了LED/TiO-PET法在降解RB5染料及其有毒副产物方面的有效性。

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