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电离辐射对头孢克洛的分解与矿化作用:动力学及自由基清除剂的影响

Decomposition and mineralization of cefaclor by ionizing radiation: kinetics and effects of the radical scavengers.

作者信息

Yu Seungho, Lee Byungjin, Lee Myunjoo, Cho Il-Hyoung, Chang Soon-Woong

机构信息

Advanced Radiation Technology Institute, Korea Atomic Energy Research Institute, Jeongeup, Jeonbuk 580-185, Republic of Korea.

出版信息

Chemosphere. 2008 May;71(11):2106-12. doi: 10.1016/j.chemosphere.2008.01.020. Epub 2008 Mar 4.

Abstract

There has been recent growing interest in the presence of antibiotics in different environmental sectors. One considerable concern is the potential development of antibiotic-resistant bacteria in the environment, even at low concentrations. Cefaclor, one of the beta-lactam antibiotics, is widely used as an antibiotic. Kinetic studies were conducted to evaluate the decomposition and mineralization of cefaclor using gamma radiation. Cefaclor, 30 mg/l, was completely degraded with 1,000 Gy of gamma radiation. At a concentration of 30 mg/l, the removal efficiency, represented by the G-value, decreased with increasing accumulated radiation dose. Batch kinetic experiments with initial aqueous concentrations of 8.9, 13.3, 20.0 and 30.0mg/l showed the decomposition of cefaclor using gamma radiation followed a pseudo first-order reaction, and the dose constant increased with lower initial concentrations. At a given radiation dose, the G-values increased with higher initial cefaclor concentrations. The experimental results using methanol and thiourea as radical scavengers indicated that ()OH radicals were more closely associated with the radiolytic decomposition of cefaclor than other radicals, such as e(aq)(-) or ()H. The radical scavenger effects were tested under O(2) and N(2)O saturations for the enhancement of the TOC percentage removal efficiencies in the radiolytic decomposition of cefaclor. Under O(2) saturation, 90% TOC removal was observed with 100,000 Gy. Oxygen is well known to play a considerable role in the degradation of organic substances with effective chain reaction pathways. According to the effective radical reactions, the enhanced TOC percentage removal efficiencies might be based on the fast conversion reactions of e(aq)(-) and ()H with O(2) into oxidizing radicals, such as O(2)(-) and HO(2)(), respectively. 100% TOC removal was obtained with N(2)O gas at 20,000 Gy, as reducing radicals, such as e(aq)(-) and ()H, are scavenged by N(2)O and converted into ()OH radicals, which have strong oxidative properties. The results of this study showed that gamma irradiation was very effective for the removal of cefaclor in aqueous solution. The use of O(2) or N(2)O, with radiation, shows promise as effective radical scavengers for enhancing the TOC or COD removal efficiencies in pharmaceutical wastewaters containing antibiotics. However, the biological toxicity and interactions between various chemicals during the radiolytic treatment, as well as treatments under conditions more representative of real wastewater will require further studies.

摘要

近年来,不同环境领域中抗生素的存在引发了越来越多的关注。一个相当令人担忧的问题是,即使在低浓度环境中,也可能会产生抗抗生素细菌。头孢克洛是β-内酰胺类抗生素之一,被广泛用作抗生素。进行了动力学研究,以评估γ辐射对头孢克洛的分解和矿化作用。30mg/l的头孢克洛在1000Gy的γ辐射下完全降解。在30mg/l的浓度下,以G值表示的去除效率随着累积辐射剂量的增加而降低。初始水溶液浓度分别为8.9、13.3、20.0和30.0mg/l的间歇动力学实验表明,γ辐射对头孢克洛的分解遵循准一级反应,剂量常数随初始浓度降低而增加。在给定的辐射剂量下,G值随头孢克洛初始浓度的升高而增加。使用甲醇和硫脲作为自由基清除剂的实验结果表明,与其他自由基(如e(aq)(-)或()H)相比,()OH自由基与头孢克洛的辐射分解关系更为密切。在O(2)和N(2)O饱和条件下测试了自由基清除剂对头孢克洛辐射分解中总有机碳(TOC)去除效率提高的影响。在O(2)饱和条件下,100000Gy的辐射可实现90%的TOC去除。众所周知,氧在具有有效链式反应途径的有机物质降解过程中起着重要作用。根据有效的自由基反应,提高的TOC去除效率可能基于e(aq)(-)和()H与O(2)分别快速转化为氧化自由基O(2)(-)和HO(2)()。在20000Gy的辐射下,使用N(2)O气体可实现100%的TOC去除,因为N(2)O清除了e(aq)(-)和()H等还原自由基,并将其转化为具有强氧化性质的()OH自由基。这项研究的结果表明,γ辐射对去除水溶液中的头孢克洛非常有效。在辐射过程中使用O(2)或N(2)O作为有效的自由基清除剂,有望提高含抗生素制药废水中TOC或化学需氧量(COD)的去除效率。然而,辐射处理过程中的生物毒性以及各种化学物质之间的相互作用,以及更接近实际废水条件下的处理,都需要进一步研究。

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