Activation of peroxymonosulfate by FeVO3-x for the degradation of carbamazepine: Vanadium mediated electron shuttle and oxygen vacancy modulated interface chemistry

• Published in: Chinese chemical letters 2024-01, Vol.35 (1), p.108580-440, Article 108580
• Main Authors: Lai, Leiduo, Zhou, Hongyu, Hong, Yichen, Luo, Mengfan, Shi, Yang, Zhang, Heng, Xiong, Zhaokun, Yao, Gang, Lai, Bo
• Format: Article
• Language: English
• Subjects: Bimetallic catalysts; Electron shuttles; Fe(III)/Fe(II) cycle; Oxygen vacancy; Peroxymonosulfate
• ISSN: 1001-8417; 1878-5964
• DOI: 10.1016/j.cclet.2023.108580

Fast Fe(III)/Fe(II) circulation in heterogeneous peroxymonosulfate (PMS) activation remains as a bottleneck issue that restricts the development of PMS based advanced oxidation processes. Herein, we proposed a facile ammonia reduction strategy and synthesized a novel FeVO3-x catalysts to activate PMS for the degradation of a typical pharmaceutical, carbamazepine (CBZ). Rapid CBZ removal could be achieved within 10 min, which outperforms most of the other iron or vanadium-based catalysts. Electron paramagnetic resonance analysis and chemical probe experiments revealed SO4•−, •OH, O2•− and high valent iron (Fe(IV)) were all generated in this system, but SO4•− and Fe(IV) primarily contributed to the degradation of CBZ. Besides, X-ray photoelectron spectroscopy and X-ray adsorption spectroscopy indicated that both the generated low-valent V provides and oxygen vacancy acted as superior electron donors and accelerated internal electron transfer via the unsaturated V−O−Fe bond. Finally, the proposed system also exhibited satisfactory performance in practical applications. This work provides a promising platform in heterogeneous PMS activation. Low-valent vanadium species could serve as efficient interior electron donors to accelerate surface Fe circulation for rapid reactive species generation. [Display omitted]