Carbamazepine degradation by heterogeneous activation of peroxymonosulfate with lanthanum cobaltite perovskite: Performance, mechanism and toxicity
Carbamazepine degradation by heterogeneous activation of peroxymonosulfate with lanthanum cobaltite perovskite: Performance, mechanism and toxicity
复制标题
钴酸镧钙钛矿异相活化过一硫酸盐降解卡马西平：性能、机制和毒性
DOI：
10.1016/j.jes.2020.01.003
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发表时间：
2020-05-01
影响因子：
6.9
通讯作者：
Chen, Jiabin
中科院分区：
文献类型：
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作者：
Guo, Huichao;Zhou, Xuefei;Chen, Jiabin
广泛使用的卡马西平（CBZ）是最持久的药物之一，并且常规废水处理的去除效率不足。采用合成的钴基钙钛矿（LaCoO 3）活化过一硫酸盐（PMS）降解CBZ。结果表明，LaCoO 3在中性pH下具有优异的PMS活化和CBZ降解性能，且钴浸出率低。FT-IR和XPS的结果证实了LaCoO 3在PMS活化过程中具有较高的结构和化学稳定性。电子自旋共振（ESR）分析表明，自由基物种的产生，如硫酸根自由基（SO 4中心点-）和羟基自由基（中心点OH）。自由基猝灭实验进一步揭示了SO 4中心点-作为CBZ氧化的主导氧化剂的责任。以SO 4-进攻烯属双键为起始步骤，通过CBZ的氧化反应，检测到10种产物。CBZ的转化沿着有羟基化、水解、环化和脱水等反应。经PMS/LaCoO 3处理后，CBZ溶液的毒性明显降低。(C)2020中国科学院生态环境科学研究中心由爱思唯尔公司出版
The widely used carbamazepine (CBZ) is one of the most persistent pharmaceuticals and suffers insufficient removal efficiency by conventional wastewater treatment. A synthesized Co-based perovskite (LaCoO3) was used to activate peroxymonosulfate (PMS) in order to degrade CBZ. Results showed that LaCoO3 exhibited an excellent performance in PMS activation and CBZ degradation at neutral pH, with low cobalt leaching. The results of FT-IR and XPS verified the high structurally and chemically stability of LaCoO3 in PMS activation. Electron spin resonance (ESR) analysis suggested the generation of radical species, such as sulfate radicals (SO4 center dot-) and hydroxyl radicals (center dot OH). Radical quenching experiments further revealed the responsibility of SO4 center dot- as the dominant oxidant for CBZ oxidation. Ten products were detected via the oxidation of CBZ, with the olefinic double bond attacked by SO4- as the initial step. Hydroxylation, hydrolysis, cyclization and dehydration were involved along the transformation of CBZ. The toxicity of CBZ solution was significantly reduced after treating by PMS/LaCoO3. (C) 2020 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.