Taghizadeh Fereshteh, Zabihi Mohammad
Chemical Engineering Faculty, Sahand University of Technology, Sahand New Town, P.O. Box 51335-1996, Tabriz, Iran.
Environ Sci Pollut Res Int. 2025 Mar;32(15):9785-9808. doi: 10.1007/s11356-025-36296-5. Epub 2025 Mar 28.
In the present study, the heterogeneous catalysts were synthesized using a facile, economical and environmentally friendly method supported on the natural mineral bentonite to degrade amoxicillin (AMX) and cephalexin (CLX) in the aqueous solutions by employing the photo-Fenton process. The characterization tests including X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscope (FESEM), energy dispersive X-ray (EDAX), transmission electron microscopy (TEM), Brunauer-Emmett-Teller (BET), ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS) and vibrating sample magnetometer (VSM) were evaluated to distinguish the physical and chemical properties of the nanocomposites. The adsorption capacity and catalytic performance of the prepared samples for the removal of AMX were investigated in order to compare the presented catalysts, in addition to the structural analysis. Among the fabricated samples, the magnetic nano-catalyst derived from two different sources of iron (ferrous sulfate and ferric nitrate) named FSF-Be was selected as the appropriate catalyst due to its high efficiency for the simultaneous degradation of CLX and AMX. Response surface method (RSM-central composite design (CCD)) was also applied to determine the effect of the operating conditions encompassing pH, initial concentration of contaminants, dosage of catalyst and hydrogen peroxide concentration for the degradation of CLX and AMX, simultaneously. The quadratic mathematical models were developed with high correlation coefficient (0.9454 and 0.9564) for the removal efficiency of AMX and CLX, respectively. Therefore, the maximum degradation efficiency of CLX and AMX was obtained to be about 96.36% and 81.61%, respectively, at the optimal conditions (pH of 3, HO concentration of 12 mM, catalyst dosage of 0.24 g/L and initial concentration of 23 mg/L) in half hour. The ozonation and the combined photo-Fenton/ozone process were investigated. The mineralization analysis illustrated that the photo-Fenton process was able to remove TOC by 73.35%, while only 2.44% of TOC removal was reached by ozonation. The degradation efficiency of CLX and AMX in the photo-Fenton/ozone system within 15 min of reaction was measured as 87.69% and 70.02%, respectively, and 61.9% mineralization was achieved in this system. However, the results showed that the photo-Fenton using FSF-Be was more efficient. The regeneration and reusability of the prepared nanocomposite was also carried out by five consecutive cycles which showed an acceptable performance in the industrial applications. The achievements demonstrated that the removal efficiency of CLX and AMX decreased about 24 and 18% after fifth cycle.
在本研究中,采用简便、经济且环保的方法,以天然矿物膨润土为载体合成了非均相催化剂,通过光芬顿工艺降解水溶液中的阿莫西林(AMX)和头孢氨苄(CLX)。进行了包括X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、场发射扫描电子显微镜(FESEM)、能量色散X射线(EDAX)、透射电子显微镜(TEM)、布鲁诺尔-埃米特-泰勒(BET)、紫外-可见漫反射光谱(UV-Vis DRS)和振动样品磁强计(VSM)在内的表征测试,以区分纳米复合材料的物理和化学性质。除了结构分析外,还研究了制备样品对AMX的吸附容量和催化性能,以比较所提出的催化剂。在制备的样品中,源自两种不同铁源(硫酸亚铁和硝酸铁)的磁性纳米催化剂FSF-Be因其对CLX和AMX的同时高效降解而被选为合适的催化剂。还应用响应面法(RSM-中心复合设计(CCD))来确定包括pH、污染物初始浓度、催化剂用量和过氧化氢浓度在内的操作条件对CLX和AMX降解的影响。分别建立了AMX和CLX去除效率的二次数学模型,相关系数较高(分别为0.9454和0.9564)。因此,在最佳条件(pH为3、HO浓度为12 mM、催化剂用量为0.24 g/L和初始浓度为23 mg/L)下,半小时内CLX和AMX的最大降解效率分别约为96.36%和81.61%。研究了臭氧化以及光芬顿/臭氧联合工艺。矿化分析表明,光芬顿工艺能够去除73.35%的总有机碳(TOC),而臭氧化仅能去除2.44%的TOC。在光芬顿/臭氧体系中反应15分钟后,CLX和AMX的降解效率分别测定为87.69%和70.02%,该体系实现了61.9%的矿化。然而,结果表明使用FSF-Be的光芬顿工艺更高效。还对制备的纳米复合材料进行了连续五个循环的再生和再利用,其在工业应用中表现出可接受的性能。结果表明,在第五个循环后,CLX和AMX的去除效率分别下降了约24%和18%。