Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China; Joint School of National University of Singapore and Tianjin University, Fuzhou International Campus, Tianjin University, Binhai New City, Fuzhou, 350207, China.
Chemosphere. 2022 Jan;287(Pt 2):132154. doi: 10.1016/j.chemosphere.2021.132154. Epub 2021 Sep 4.
Designing catalysts that can effectively activate oxygen and hydrogen peroxide is a huge challenge in electro-Fenton (EF) process. Considering the superior ability of electrons transport and activation of HO, ceria encapsulated with N, P-codoped carbon material was a promising catalyst for EF reaction. Herein, CeO-NPC (where T and X represented the calcination temperature and the initial mass of CeO, respectively) materials were synthesized via pyrolysis process and used as catalysts to degrade ciprofloxacin (CIP) in EF process. The results indicated that CeO-NPC catalyst had good degradation performance under the optimal conditions. Compared with CeO and CeO-NC catalysts, CeO-NPC catalyst had more content of graphite N and more oxygen vacancies, which were beneficial to activation of oxygen and hydrogen peroxide. Scavenging experiments and electron paramagnetic resonance analysis confirmed ·O and ·OH were the main reactive oxygen species in the CIP degradation process. And three logical degradation routes of CIP were given. In addition, CeO-NPC catalyst still had good stability after three times of continuous operation, and presented good universality for the treatment of a variety of antibiotic wastewaters. Finally, a convincing mechanism in the EF system with CeO-NPC for CIP degradation was proposed.
设计能够有效激活氧气和过氧化氢的催化剂是电芬顿（EF）过程中的一个巨大挑战。考虑到电子传输和 HO 激活的优越能力，用 N、P 共掺杂碳材料封装的氧化铈是 EF 反应的一种很有前途的催化剂。本文通过热解过程合成了 CeO-NPC（其中 T 和 X 分别代表煅烧温度和 CeO 的初始质量）材料，并将其用作催化剂在 EF 过程中降解环丙沙星（CIP）。结果表明，CeO-NPC 催化剂在最佳条件下具有良好的降解性能。与 CeO 和 CeO-NC 催化剂相比，CeO-NPC 催化剂具有更多的石墨 N 和更多的氧空位，这有利于氧气和过氧化氢的活化。猝灭实验和电子顺磁共振分析证实，·O 和·OH 是 CIP 降解过程中的主要活性氧物质。并给出了 CIP 的三种逻辑降解途径。此外，CeO-NPC 催化剂在三次连续运行后仍具有良好的稳定性，对多种抗生素废水的处理具有良好的通用性。最后，提出了 CeO-NPC 在 EF 体系中用于 CIP 降解的令人信服的机制。
