Bodaghifard Mohammad Ali, Hamidinasab Mahdia, Bayat Pegah
Department of Chemistry, Faculty of Science, Arak University, Arak, 38156-88138, Iran.
Institute of Nanosciences and Nanotechnology, Arak University, Arak, 38156-88138, Iran.
Environ Sci Pollut Res Int. 2023 Apr;30(20):57821-57832. doi: 10.1007/s11356-023-26614-0. Epub 2023 Mar 27.
Magnetic nanoparticles surrounded with a silica shell are useful materials to immobilize active agents on their surface. Here, a heteropolyacid-functionalized hybrid nanomaterial (NiFeO@SiO-DETA@POM) was prepared and characterized by X-ray powder diffraction patterns (XRD), Fourier-transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA/DTG), vibrating sample magnetometer (VSM), the field emission scanning electron microscopy (FE-SEM), and the electron-dispersive X-ray spectroscopy (EDS). The synthesized hybrid nanostructure was used as a solid nanocatalyst in oxidative desulfurization (ODS) of real fuel and simulated gasoline samples. The ODS process of benzothiophene (BT) and dibenzothiophene (DBT) as model compounds in the presence of NiFeO@SiO-DETA@POM and by using urea-hydrogen peroxide/acetic acid as a safer oxidizing agent was investigated. A good result was obtained by removing 97% of benzothiophene and 98% of dibenzothiophene. Also, 96% of the sulfur compounds were eliminated when the ODS process was tested on a real crude oil sample (600 ppm) under an optimized dosage of nanocatalyst, urea-hydrogen peroxide/acetic acid (0.1 g, 1 g/4 ml) at 50 ºC for 60 min. NiFeO@SiO-DETA@POM could be recycled for five consecutive oxidation runs without significant deterioration in its catalytic activity. The UHP's safety and efficiency as an oxidant, high removal efficacy, short transformation times, easy workup procedure, catalyst reusability, simple separation of nanocatalyst, green conditions, and environmental compatibility and sustainability. The obtained results prove that NiFeO@SiO-DETA@POM is a suitable and efficient hybrid catalyst for the oxidative desulfurization of simulated and real fuels.
包覆有二氧化硅壳层的磁性纳米颗粒是将活性剂固定在其表面的有用材料。在此,制备了一种杂多酸功能化的杂化纳米材料(NiFeO@SiO-DETA@POM),并通过X射线粉末衍射图谱(XRD)、傅里叶变换红外光谱(FT-IR)、热重分析(TGA/DTG)、振动样品磁强计(VSM)、场发射扫描电子显微镜(FE-SEM)和电子能谱X射线光谱(EDS)对其进行了表征。合成的杂化纳米结构被用作实际燃料和模拟汽油样品氧化脱硫(ODS)中的固体纳米催化剂。研究了在NiFeO@SiO-DETA@POM存在下,以尿素-过氧化氢/乙酸作为更安全的氧化剂,将苯并噻吩(BT)和二苯并噻吩(DBT)作为模型化合物的ODS过程。通过去除97%的苯并噻吩和98%的二苯并噻吩获得了良好的结果。此外,在优化的纳米催化剂、尿素-过氧化氢/乙酸(0.1 g,1 g/4 ml)用量下,于50℃处理60分钟,对实际原油样品(600 ppm)进行ODS过程测试时,96%的硫化合物被去除。NiFeO@SiO-DETA@POM可以连续循环使用五次氧化运行,其催化活性没有明显下降。超氧尿素作为氧化剂的安全性和效率、高去除效率、短转化时间、简单的后处理程序、催化剂可重复使用性、纳米催化剂的简单分离、绿色条件以及环境兼容性和可持续性。所得结果证明,NiFeO@SiO-DETA@POM是用于模拟和实际燃料氧化脱硫的合适且高效的杂化催化剂。