4.7 Article

Facile synthesis of oxygen vacancies enriched α-Fe2O3 for peroxymonosulfate activation: A non-radical process for sulfamethoxazole degradation

期刊

JOURNAL OF HAZARDOUS MATERIALS
卷 419, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.jhazmat.2021.126447

关键词

Peroxymonosulfate; Singlet oxygen; Oxygen vacancy; Sulfamethoxazole; Iron-based catalyst

资金

  1. National Natural Science Foundation of China [51822806, 41671468]
  2. Qing Lan Project of Jiangsu Province
  3. Fundamental Research Funds for the Central Universities

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This study prepared oxygen vacancies-enriched alpha-Fe2O3 as a catalyst for PMS activation by thermally treating goethite, showing excellent catalytic activity. The concentration of oxygen vacancies was found to be positively correlated with the degradation rate of SMX, with singlet oxygen identified as the predominant reactive oxygen species. The study comprehensively investigated the factors affecting SMX degradation and proposed possible degradation pathways in the alpha-Fe2O3/PMS system.
Hematite (alpha-Fe2O3) has been commonly used as an eco-friendly catalyst for peroxymonosulfate (PMS) to generate free radicals (SO4 center dot- and/or center dot OH). However, the activation efficiency of PMS relies heavily on the conversion of Fe(III) to Fe(II) that is slow and rate-limiting. In this study, oxygen vacancies enriched alpha-Fe2O3 was prepared from thermally treated goethite (alpha-FeOOH) and employed as a PMS activator. Systematic characterization demonstrated that alpha-Fe2O3 with most abundant oxygen vacancies could be obtained by heating alpha-FeOOH at 300 degrees C. The as-prepared alpha-Fe2O3 exhibited excellent catalytic activity in activation of PMS for oxidation of sulfamethoxazole (SMX, k = 0.04 min(-1)). The SMX degradation rate was found to be positively correlated with the concentration of oxygen vacancies. Quenching experiments, EPR, LC/MS and XPS analysis revealed that singlet oxygen (O-1(2)) was the predominant reactive oxygen species. The effects of pH, PMS dosage, catalyst loading, temperature, and anions on SMX degradation were comprehensively investigated. Moreover, the plausible degradation pathways of SMX in the alpha-Fe2O3/PMS system were proposed. This work not only provides a valuable insight into the mechanism of PMS activation by alpha-Fe2O3 but also establishes a new strategy for the design of more efficient and practical iron-based catalyst for PMS activation.

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