Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-06-08 , DOI: 10.1016/j.jhazmat.2021.126360 Xinlu Yang 1 , Xinyu Xie 1 , Siqi Li 2 , Wenxuan Zhang 1 , Xiaodan Zhang 2 , Hongxiang Chai 1 , Yuming Huang 2
Herein, we reported the design and fabrication of polyoxometalates coupling metal-organic framework (POM@MOF) hybrids derived hierarchical hollow Mo/Co bimetal oxides nanocages (Mo/Co HHBONs) for the peroxymonosulfate (PMS) activation to degrade levofloxacin (Lev). The Mo/Co HHBONs are hollow nanocages with high specific-surface areas and hierarchical micropores, mesopores, and macropores. In addition to compositional modulation, polyoxometalate (H3PMo12O40·nH2O) exhibited striking effect on the textural properties of Mo/Co HHBONs. The Mo/Co HHBONs had outstanding catalytic activity with first order-kinetics that were 6 − 10 times higher those previously reported. They exhibited good adaptability over a pH range of 3 − 11, as well as excellent universality and reusability. By altering the surface porosity, electronic structure, and oxygen vacancies of Co3O4, hetero-metal Mo doping induced Mo/Co HHBONs significantly promote the generation of reactive oxygen species, including •OH, SO4•−, O2•−, and 1O2. Density functional theory indicated that Mo/Co HHBONs had better adsorption, enhanced electron-transfer abilities, and a longer O-O bond length than did Co3O4, for improved catalytic reactivity. This research provides a new strategy to design the POM@MOF hybrids derived hierarchical hollow nanocages with highly PMS activating capacity for the removal of antibiotics and other refractory contaminants.
中文翻译:
POM@MOF 杂化衍生的分层空心 Mo/Co 双金属氧化物纳米笼有效激活过硫酸盐降解左氧氟沙星
在此,我们报道了多金属氧酸盐偶联金属-有机框架 (POM@MOF) 杂化物的设计和制造,衍生出分层空心 Mo/Co 双金属氧化物纳米笼 (Mo/Co HHBONs),用于过硫酸盐 (PMS) 活化降解左氧氟沙星 (Lev)。Mo/Co HHBONs 是具有高比表面积和分级微孔、中孔和大孔的中空纳米笼。除了成分调制外,多金属氧酸盐 (H 3 PMo 12 O 40 ·nH 2O) 对 Mo/Co HHBONs 的结构特性表现出显着影响。Mo/Co HHBONs 具有出色的催化活性,一级动力学是先前报道的 6-10 倍。它们在 3 - 11 的 pH 范围内表现出良好的适应性,以及出色的通用性和可重用性。通过改变 Co 3 O 4的表面孔隙率、电子结构和氧空位,异质金属 Mo 掺杂诱导的 Mo/Co HHBONs 显着促进了活性氧物质的产生,包括• OH、SO 4 •-、O 2 •- , 和1 O 2. 密度泛函理论表明,与Co 3 O 4相比,Mo/Co HHBONs 具有更好的吸附性、增强的电子转移能力和更长的OO 键长,以提高催化反应性。该研究为设计具有高度 PMS 活化能力的 POM@MOF 杂化物衍生的分级空心纳米笼提供了一种新策略,以去除抗生素和其他难降解的污染物。