1. Enhanced removal of As(iii) by manganese-doped defective UiO-66 coupled peroxymonosulfate: multiple reactive oxygen species and system stabilityElectronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d4en00194j
- Author
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Xie, Zihao, He, Qingyun, Liu, Shaobo, Huang, Xinyi, Dai, Mingyang, Chen, Qiang, Sun, Ang, Ye, Jian, Tan, Xiaofei, and Xu, Weihua
- Abstract
Structurally defective UiO-66 has garnered significant interest due to its remarkable performance in the domains of adsorption and catalysis. In this research, the successful synthesis of Mn-doped defective UiO-66 (Mn1D40UiO-66) was confirmed by XRD and FTIR characterization. More than 95% of As(iii) (C0= 1.1 mg L−1) was removed in 1 h (Ccatalyst= 0.2 g L−1, CPMS= 0.1 mM). Compared with the original UiO-66, when coupled with peroxymonosulfate (PMS), Mn1D40UiO-66 accelerated the generation of reactive oxygen species (ROS), resulting in an increase in As(iii) removal efficiency by about 50%. XPS spectra and EXAFS spectra indicated that As(iii) adsorbed in the Mn1D40UiO-66/PMS system was fully oxidized to As(v) and the adsorption was attributed to As–O–Zr coordination. Several types of ROS (·OH, SO4−, and O2−) generated by PMS activation acted collectively on As(iii) oxidation, so a single ROS scavenger did not have a marked inhibitory effect on As(iii) removal. In addition, the system maintained efficiency over a broad pH range (3–11), and retained an arsenic removal rate higher than 89.8% even in the presence of high concentrations of several anions (SO42−/Cl−/NO3−, 10 mM). Meanwhile, 99.3% of the As(iii) could be removed by Mn1D40UiO-66 at extremely high humic acid concentrations (100 mg L−1). Due to the excellent stability of the material, only trace amounts of metal leaching were detected (Mn ion ≤ 3 μg L−1) during the whole experiment. The whole oxidation and adsorption process demonstrated excellent anti-interference ability and stability. This study shows the great potential of transition metal doped defective metal–organic frameworks in the field of adsorption and catalysis and provides a novel idea for the high-efficiency management of As(iii) pollution in water environments.
- Published
- 2024
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