Journal
CHEMICAL ENGINEERING JOURNAL
Volume 400, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2020.125872
Keywords
g-C3N4; beta-FeOOH; Peroxymonosulfate activation; Solar irradiation; Deep oxidation
Categories
Funding
- National Natural Science Foundation of China [51133006, 51103133]
- Zhejiang Provincial Natural Science Foundation of China [Q19E030051]
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Peroxymonosulfate (PMS) activation with the generation of strongly oxidizing hydroxyl radicals (center dot OH) and sulfate radicals (SO4 center dot-) has attracted widespread attention for the elimination of organic contaminants. However, the design of an eco-friendly catalytic system with high mineralization rate and high stability remains a challenge. Here, an iron-based photocatalyst (beta-FeOOH@g-C3N4) for the activation of PMS was prepared by a cyclic microwave-assisted reaction, whereby Fe3+ was introduced at the nitrogen sites of g-C3N4, resulting in in situ growth and a uniform distribution of nano-beta-FeOOH thereon. beta-FeOOH@g-C3N4 maintained high catalytic activity after acid treatment or repeated tests, demonstrating excellent stability and reusability. Moreover, compared with the catalytic systems with beta-FeOOH or g-C3N4 alone, the catalytic activity of beta-FeOOH@g-C3N4 was increased 5-10 times for the catalytic oxidation of carbamazepine (CBZ) and other emerging contaminants under solar irradiation. Importantly, the CBZ mineralization rate with the beta-FeOOH@g-C3N4/PMS system under solar irradiation was as high as 92%. From the results of electron paramagnetic resonance spectroscopy and radical trapping experiments, large amounts of O-2(center dot-), O-1(2), and Fe-V = O are present at the beginning of the reaction, which contribute to the rapid oxidative removal of CBZ, while SO4 center dot- and (OH)-O-center dot contribute to the deep oxidation, leading to a significantly enhanced total organic carbon (TOC) removal efficiency. This work provides an alternative method for the design of a highly efficient and stable catalyst for PMS activation to eliminate emerging contaminants.
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