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在改性石墨毡阴极电芬顿体系中,土霉素降解的动力学和机制。

Kinetics and mechanisms of oxytetracycline degradation in an electro-Fenton system with a modified graphite felt cathode.

机构信息

School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China.

Guangdong Yikangsheng Environmental Science and Technology Limited Company, Yunfu, 527400, China.

出版信息

J Environ Manage. 2020 Mar 1;257:109968. doi: 10.1016/j.jenvman.2019.109968. Epub 2019 Dec 23.

Abstract

The removal of trace antibiotics from the aquatic environment has received great interest. In this investigation, NaOH activated graphite felt (NaOH-GF) was characterized by multiple-methods, including scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), contact angle, linear sweep voltammetry (LSV) and electron paramagnetic resonance (EPR). The NaOH-GF was then used as the cathode in the electro-Fenton process for oxytetracycline (OTC) degradation, the experiment was carried out in an undivided and light-proof beaker with a Pt anode and a NaOH-GF cathode at pH 3. The results showed that the modification with NaOH enhanced the antibiotics degradation efficiency of graphite felt by increasing the oxygen reduction capacity and hydroxyl radicals yielding rate. Complete OTC removal was achieved at 5.17 mA cm after 40, 60 and 90 s with initial OTC concentration of 22, 44, and 66 μM, respectively. With an initial OTC concentration of 44 μM, after 30 min the removal rates of chemical oxygen demand (COD) by Raw-GF and NaOH-GF were 59.18% and 83.75%, respectively. The proposed degradation mechanism of OTC was an EF process, which consisted of hydroxylation, secondary alcohol oxidation, demethylation, decarbonylation, dehydration and deamination. This study demonstrates that NaOH activated GF cathode possesses high degradation capacity and good stability. It provides insight into the removal of non-biodegradable antibiotics and may shed light on future to its practical application.

摘要

从水环境中去除痕量抗生素受到了广泛关注。在这项研究中,采用多种方法对 NaOH 活化石墨毡(NaOH-GF)进行了表征,包括扫描电子显微镜(SEM)、X 射线光电子能谱(XPS)、接触角、线性扫描伏安法(LSV)和电子顺磁共振(EPR)。然后,将 NaOH-GF 用作电芬顿工艺中降解土霉素(OTC)的阴极,在一个不分隔且避光的烧杯中进行实验,使用 Pt 阳极和 NaOH-GF 阴极,pH 值为 3。结果表明,NaOH 的修饰通过增加氧还原能力和羟基自由基生成速率,提高了石墨毡的抗生素降解效率。当初始 OTC 浓度分别为 22、44 和 66 μM 时,在 40、60 和 90 s 后,电流密度为 5.17 mA cm时,OTC 可完全去除。当初始 OTC 浓度为 44 μM 时,Raw-GF 和 NaOH-GF 对化学需氧量(COD)的去除率分别为 59.18%和 83.75%,反应 30 min 后。OTC 的降解机制为 EF 过程,包括羟化、仲醇氧化、脱甲基、脱羰基、脱水和脱氨。该研究表明,NaOH 活化 GF 阴极具有较高的降解能力和良好的稳定性。它为去除不可生物降解的抗生素提供了新的思路,并可能为其实际应用提供启示。

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