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Novel activation of peroxymonosulfate by an easily recyclable VC@Fe3O4 nanoparticles for enhanced degradation of sulfadiazine

Journal 2019 · IF 8.355 · 发表于 2019 年 1 月 24 日
作者: Chaoqun Tan,Xu Lu,Xinxin Cui,Xinchi Jian,Zhixian Hu,Yujie Dong,Xiaoyu Liu,Juan Huang,Ling Deng
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摘要

An easily recyclable nanocomposite ascorbic acid-modified Fe 3 O 4 (VC@Fe 3 O 4 ) was synthesized, characterized, and evaluated as a green heterogeneous catalyst for activation of peroxymonosulfate (PMS). The structures of fresh and used VC@Fe 3 O 4 were well characterized by TEM, XRD, FTIR, and XPS. The catalytic activity comparison between Fe 3 O 4 and VC@Fe 3 O 4 was performed under different parameters for depletion of sulfadiazine (SD). Additionally, scavenging tests and in-situ electron paramagnetic resonance (EPR) tests were applied to discern the primary radicals generated in the VC@Fe 3 O 4 /PMS system. The results indicate that the VC@Fe 3 O 4 possesses a higher catalytic activity towards PMS compared with Fe 3 O 4 for SD removal, and the observed pseudo first rate constant ( k obs ) were 7.24 × 10 −2  min −1 for the VC@Fe 3 O 4 /PMS system and 1.05 × 10 −2  min −1 for the Fe 3 O 4 /PMS system, correspondingly. 56.6% SD removal efficiency was obtained with 0.3 mM PMS and 0.8 g/L VC@Fe 3 O 4 under pH 7.0. A large amount of hydroxyl radicals (OH ) and a few number of sulfate radicals (SO 4 − ) were discerned by the hyperfine splitting constant values and scavenging results. Mechanisms on the peroxymonosulfate activation and radical generation in the VC@Fe 3 O 4 /PMS system were supposed. Results indicate that VC would obviously boost the cycle of Fe 2+ -Fe 3+ on surface of VC@Fe 3 O 4 nanoparticles and newly generated Fe 2+ can continuously be consumed to activate PMS, which is answer for the rapid generation of reactive radicals (OH , SO 4 − ). At last, mineralization and degradation pathway were also investigated. The findings of this study suggest that VC@Fe 3 O 4 is a novel effective catalyst in activation of peroxymonosulfate under neutral pHs.

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