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Rapid Hydrolysis of Penicillin Antibiotics Mediated by Adsorbed Zinc on Goethite Surfaces
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2019-08-28 , DOI: 10.1021/acs.est.9b02666
Feng Sheng 1 , Jingyi Ling 1 , Chao Wang 1 , Xin Jin 1 , Xueyuan Gu 1 , Hong Li 2 , Jiating Zhao 2 , Yujun Wang 3 , Cheng Gu 1
Affiliation  

The soil environment is an important sink for penicillin antibiotics released from animal manure and wastewater, but the mineral-catalyzed transformation of penicillins in soil has not been well studied. To simulate this environmental process, we systematically investigated the behavior of penicillin G and amoxicillin, the two most widely-used penicillin antibiotics, in the presence of goethite and metal ions. The results demonstrated that Zn ions significantly promoted the hydrolysis of penicillins in goethite suspensions, as evidenced by the degradation rate nearly 3 orders of magnitude higher than that of the non-Zn-containing control. The spectroscopic analysis indicated that the specific complexation between penicillins, adsorbed Zn, and goethite was responsible for the enhanced degradation. Metastable interactions, involving hydrogen bonds between carbonyl groups in the β-lactam ring and the double/triple hydroxyl groups on goethite surface, and coordination bonding between carboxyl groups and surface irons were proposed to stabilize the ternary reaction intermediates. Moreover, the surface zinc-hydroxide might act as powerful nucleophile to rapidly rupture the β-lactam ring in penicillins. This study is among the first to identify the synergic roles of Zn ion and goethite in facilitating penicillin degradation and provides insights into β-lactam antibiotics to assess their environmental risk in soil.

中文翻译:

针铁矿表面吸附锌介导的青霉素类抗生素快速水解

土壤环境是从动物粪便和废水中释放出青霉素抗生素的重要水槽,但土壤中青霉素的矿物催化转化尚未得到很好的研究。为了模拟这种环境过程,我们系统地研究了在针铁矿和金属离子存在下青霉素G和阿莫西林这两种使用最广泛的青霉素抗生素的行为。结果表明,Zn离子显着促进针铁矿悬浮液中青霉素的水解,其降解速率比不含锌的对照高近3个数量级。光谱分析表明,青霉素,吸附的锌和针铁矿之间的特定络合是降解增强的原因。亚稳态相互作用 为了稳定三元反应中间体,提出了在β-内酰胺环上的羰基与针铁矿表面上的双/三羟基之间存在氢键,并在羧基和表面铁之间进行配位键化。此外,表面氢氧化锌可能充当强亲核试剂,以快速破坏青霉素中的β-内酰胺环。这项研究是首次确定Zn离子和针铁矿在促进青霉素降解中的协同作用,并为深入了解β-内酰胺类抗生素在土壤中的环境风险提供了见识。表面氢氧化锌可能会充当强大的亲核试剂,从而使青霉素中的β-内酰胺环迅速断裂。这项研究是首次确定Zn离子和针铁矿在促进青霉素降解中的协同作用,并为深入了解β-内酰胺类抗生素在土壤中的环境风险提供了见识。表面氢氧化锌可能会充当强大的亲核试剂,从而使青霉素中的β-内酰胺环迅速断裂。这项研究是首次确定Zn离子和针铁矿在促进青霉素降解中的协同作用,并为深入了解β-内酰胺类抗生素在土壤中的环境风险提供了见识。
更新日期:2019-08-28
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