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通过有机和无机添加剂强化超声化学降解亲水性有机污染物。

Intensifying the sonochemical degradation of hydrophilic organic contaminants by organic and inorganic additives.

机构信息

Grupo de Investigación en Remediación Ambiental y Biocatálisis (GIRAB), Instituto de Química, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombia.

Grupo de Investigación en Remediación Ambiental y Biocatálisis (GIRAB), Instituto de Química, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombia; Grupo de Catalizadores y Adsorbentes (CATALAD), Instituto de Química, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 # 52-21, Medellín, Colombia.

出版信息

J Environ Manage. 2024 Aug;366:121930. doi: 10.1016/j.jenvman.2024.121930. Epub 2024 Jul 24.

Abstract

The sonochemical system is highly effective at degrading hydrophobic substances but has limitations when it comes to eliminating hydrophilic compounds. This study examines the impact of organic and inorganic additives on improving the sonochemical degradation of hydrophilic pollutants in water. The effects of adding an organic substance (CCl) and two inorganic ions (Fe and HCO) were tested. The treatment was focused on a representative hydrophilic antibiotic, cefadroxil (CDX). Initially, the sonodegradation of CDX without additives was assessed and compared with two reference pollutants more hydrophobic than CDX: dicloxacillin (DCX) and methyl orange (MO). The results highlighted the limitations of ultrasound alone in degrading CDX. Subsequently, the impact of the additives on enhancing the removal of this recalcitrant pollutant was evaluated at two frequencies (375 and 990 kHz). A significant improvement in the CDX degradation was observed with the presence of CCl and Fe at both frequencies. Increasing CCl concentration led to greater CDX elimination, whereas a high Fe concentration had detrimental effects. To identify the reactive sites on CDX towards the species generated with the additives, theoretical calculations (i.e. Fukui indices and HOMO-LUMO gaps) were performed. These analyses indicated that the β-lactam and dihydrothiazine rings on CDX are highly reactive towards oxidizing species. This research enhances our understanding of the relationship between the structural characteristics of contaminants and the sonochemical frequency in the action of additives having diverse nature.

摘要

声化学体系在降解疏水性物质方面非常有效,但在消除亲水性化合物方面存在局限性。本研究考察了有机和无机添加剂对改善水中亲水性污染物的声化学降解的影响。测试了添加一种有机物质(CCl)和两种无机离子(Fe 和 HCO)的效果。处理集中在一种代表性的亲水性抗生素,头孢羟氨苄(CDX)上。首先,评估了没有添加剂的 CDX 的声降解,并将其与两种疏水性比 CDX 更高的参考污染物:双氯西林(DCX)和甲基橙(MO)进行了比较。结果突出了单独使用超声波降解 CDX 的局限性。随后,在两种频率(375 和 990 kHz)下评估了添加剂对增强这种难降解污染物去除的影响。在两种频率下,添加 CCl 和 Fe 都显著提高了 CDX 的降解。增加 CCl 浓度会导致 CDX 的去除率更高,而高浓度的 Fe 则会产生不利影响。为了确定 CDX 对添加剂生成的物质的反应活性位点,进行了理论计算(即福井指数和 HOMO-LUMO 间隙)。这些分析表明,CDX 上的β-内酰胺和二氢噻嗪环对氧化物种具有很高的反应活性。这项研究提高了我们对污染物结构特征与添加剂性质多样的声化学频率之间关系的理解。

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