Department of Civil Engineering, Kyung Hee University , 1732 Deokyoung-daero, Yongin-si, Gyeonggi-do 17104, Republic of Korea.
ACS Appl Mater Interfaces. 2017 Aug 30;9(34):28508-28518. doi: 10.1021/acsami.7b07658. Epub 2017 Aug 16.
Recently, yolk-shell structured materials with active metal cores have received considerable attention in heterogeneous Fenton-like systems, which have excellent catalytic performance. In this study, we initially attempted the nonsacrificial template synthesis of yolk-shell structured nanoparticles with magnetite cores encapsulated in a mesoporous silica shell (FeO@SiO) via a modified sol-gel process and then evaluated their catalytic activity for acetaminophen degradation in Fenton-like systems. Second, copper nanoparticles were decorated on the surface of the FeO@SiO microspheres (FeO@SiO@Cu) to enhance the catalytic activity. The morphological, structural, and physicochemical properties of the prepared materials were characterized via X-ray diffraction, X-ray photoelectron spectroscopy, field emission scanning electron microscopy, field emission transmission electron microscopy, nitrogen adsorption-desorption isotherms, specific surface area, ζ-potential, magnetic properties, and Fourier transform infrared spectroscopy. The results demonstrated a successful fabrication of the targeted materials. The yolk-shell structured materials possess a spherical morphology with an active core, protective shell, and hollow void. The FeO@SiO and FeO@SiO@Cu variants showed acetaminophen removal rates significantly higher compared to those of their counterparts, i.e., the FeO and FeO@Cu core-shell structures. FeO@SiO@Cu showed that the copper nanoparticles were firmly immobilized on the mesoporous silica shell, dramatically improving the catalytic performance. Both the yolk-shell structured FeO@SiO and FeO@SiO@Cu exhibited good separation and satisfactory regeneration properties, which could be recycled six times without any obvious decline in catalytic activity. Overall, the results of this study suggested that FeO@SiO and FeO@SiO@Cu yolk-shell nanostructures could be promising catalysts for a heterogeneous Fenton-like system by which the removal of emerging contaminants can be greatly improved.
最近，具有活性金属核的蛋黄壳结构材料在非均相类 Fenton 体系中受到了相当大的关注，具有优异的催化性能。在这项研究中，我们最初尝试通过改进的溶胶-凝胶法，非牺牲模板合成具有磁性核的介孔硅壳（FeO@SiO）包裹的蛋黄壳结构纳米粒子（FeO@SiO），然后评估它们在类 Fenton 体系中降解对乙酰氨基酚的催化活性。其次，在 FeO@SiO 微球表面上修饰铜纳米粒子（FeO@SiO@Cu）以提高催化活性。通过 X 射线衍射、X 射线光电子能谱、场发射扫描电子显微镜、场发射透射电子显微镜、氮气吸附-脱附等温线、比表面积、ζ-电位、磁性和傅里叶变换红外光谱对制备材料的形态、结构和物理化学性质进行了表征。结果表明成功制备了目标材料。蛋黄壳结构材料具有球形形貌，具有活性核、保护壳和中空空隙。与 FeO 和 FeO@Cu 核壳结构相比，FeO@SiO 和 FeO@SiO@Cu 变体表现出更高的对乙酰氨基酚去除率。FeO@SiO@Cu 表明铜纳米粒子牢固地固定在介孔硅壳上，极大地提高了催化性能。FeO@SiO 和 FeO@SiO@Cu 的蛋黄壳结构都表现出良好的分离和令人满意的再生性能，可以回收六次而催化活性没有明显下降。总体而言，这项研究的结果表明，FeO@SiO 和 FeO@SiO@Cu 蛋黄壳纳米结构可以作为非均相类 Fenton 体系的有前途的催化剂，极大地提高了新兴污染物的去除率。
