Rapid and long-lasting acceleration of zero-valent iron nanoparticles@Ti3C2-based MXene/peroxymonosulfate oxidation with bi-active centers toward ranitidine removal?

Journal of Materials Chemistry A Pub Date: 2021-04-20 DOI: 10.1039/D1TA02046C

Abstract

Advanced oxidation processes (AOPs) can effectively degrade ranitidine, a pharmaceutical that is a typical precursor of nitrosamine dimethylamine (NDMA), an extremely potent human carcinogen. Herein, novel magnetic Ti3C2-based MXene nanosheets decorated with nanoscale zero-valent iron particles (nZVIPs@Ti3C2 nanosheets) were synthesized to boost catalytic peroxymonosulfate (PMS) activation, exhibiting remarkable reactivity and stability for the rapid removal of ranitidine under mild conditions. The response surface methodology (RSM) confirmed that the initial solution pH and PMS dosage were the main factors affecting the heterogeneous oxidation process. The long-lasting catalytic activity was mainly attributed to the rapid charge transfer between dual electron-rich active centers (≡Fe and ≡Ti), with SO4˙? and HO˙ derived from PMS activation being responsible for ranitidine degradation, among which SO4˙? was the major contributor. Density functional theory (DFT) calculations also confirmed that the as-synthesized nZVIPs@Ti3C2 nanosheets provided bi-active centers for PMS activation, and this process triggered a series of thermodynamically favorable reactions. This study demonstrates a recyclable oxidation method for the rapid removal of ranitidine, which may be applicable to the degradation of other challenging pollutants.

Graphical abstract: Rapid and long-lasting acceleration of zero-valent iron nanoparticles@Ti3C2-based MXene/peroxymonosulfate oxidation with bi-active centers toward ranitidine removal
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