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溶液中锰铜氧化物/磁铁矿催化臭氧化氯霉素:经验动力学模型、降解途径、催化机制和抗菌活性。

Catalytic ozonation of chloramphenicol with manganese-copper oxides/maghemite in solution: Empirical kinetics model, degradation pathway, catalytic mechanism, and antibacterial activity.

机构信息

Center for Environment and Water Resource, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, PR China; Key Laboratory of Hunan Province for Water Environment and Agriculture Product Safety, Changsha, 410083, PR China.

Center for Environment and Water Resource, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, PR China; Key Laboratory of Hunan Province for Water Environment and Agriculture Product Safety, Changsha, 410083, PR China.

出版信息

J Environ Manage. 2022 Jan 15;302(Pt A):114043. doi: 10.1016/j.jenvman.2021.114043. Epub 2021 Nov 1.

Abstract

The composite material of manganese-copper oxide/maghemite (MnCuO/γ-FeO) was synthesized by the co-precipitation-calcination method. With the initial concentration of 0.2 g/L MnCuO/γ-FeO and 10 mg/L O, the chloramphenicol (CAP, 10 mg/L) could be completely degraded, which was about 2.22 times of that treated with ozonation alone. The contribution of O and hydroxyl radical (•OH) for CAP degradation in the catalytic process was 6.9% and 93.1%, respectively. According to the effects of catalyst dosage, ozone dosage, and pH on the catalytic performance of MnCuO/γ-FeO, a predictive empirical model was developed for the ozonation with the MnCuO/γ-FeO system. The HCO/CO and phosphates in solution could inhibit the degradation of CAP with the inhibition ratios 8.45% and 13.8%, respectively. The HCO/CO could compete with CAP and react with •OH, and the phosphates were considered as poisons for catalysts by blocking the surface active sites to inhibit ozone decomposition. The intermediates and possible degradation pathways were detected and proposed. The catalytic ozonation could effectively control the toxicity of the treated solution, but the toxicity was still not negligible. Furthermore, MnCuO/γ-FeO could be easily and efficiently separated from the reaction system with an external magnet, and it possessed excellent reusability and stability.

摘要

采用共沉淀-煅烧法合成了氧化锰-氧化铜/磁赤铁矿(MnCuO/γ-FeO)复合材料。在 MnCuO/γ-FeO 初始浓度为 0.2 g/L 和 O 初始浓度为 10 mg/L 的条件下,氯霉素(CAP,10 mg/L)可完全降解,这大约是单独臭氧氧化的 2.22 倍。在催化过程中,O 和羟基自由基(•OH)对 CAP 降解的贡献分别为 6.9%和 93.1%。根据催化剂用量、臭氧用量和 pH 值对 MnCuO/γ-FeO 催化性能的影响,建立了 MnCuO/γ-FeO 体系臭氧氧化的预测经验模型。溶液中的 HCO/CO 和磷酸盐分别对 CAP 的降解抑制率为 8.45%和 13.8%。HCO/CO 可以与 CAP 竞争并与•OH 反应,而磷酸盐通过阻塞表面活性位点来抑制臭氧分解,被认为是催化剂的毒物。检测并提出了中间产物和可能的降解途径。催化臭氧氧化可以有效地控制处理溶液的毒性,但毒性仍然不可忽视。此外,MnCuO/γ-FeO 可以很容易地用外部磁铁从反应体系中分离出来,并且具有优异的可重复使用性和稳定性。

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