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Transformation of m-aminophenol by birnessite (δ-MnO2) mediated oxidative processes: Reaction kinetics, pathways and toxicity assessment.
Environmental Pollution ( IF 7.6 ) Pub Date : 2019-10-19 , DOI: 10.1016/j.envpol.2019.113408
Wenqian Huang 1 , Guowei Wu 1 , Hong Xiao 1 , Haiyan Song 2 , Shuzhao Gan 1 , Shuhong Ruan 1 , Zhihong Gao 1 , Jianzhong Song 3
Affiliation  

The m-aminophenol (m-AP) is a widely used industrial chemical, which enters water, soils, and sediments with waste emissions. A common soil metal oxide, birnessite (δ-MnO2), was found to mediate the transformation of m-AP with fast rates under acidic conditions. Because of the highly complexity of the m-AP transformation, mechanism-based models were taken to fit the transformation kinetic process of m-AP. The results indicated that the transformation of m-AP with δ-MnO2 could be described by precursor complex formation rate-limiting model. The oxidative transformation of m-AP on the surface of δ-MnO2 was highly dependent on reactant concentrations, pH, temperature, and other co-solutes. The UV-VIS absorbance and mass spectra analysis indicated that the pathway leading to m-AP transformation may be the polymerization through the coupling reaction. The m-AP radicals were likely to be coupled by the covalent bonding between unsubstituted C2, C4 or C6 atoms in the m-AP aromatic rings to form oligomers as revealed by the results of activation energy and mass spectra. Furthermore, the toxicity assessment of the transformation productions indicated that the toxicity of m-AP to the E. coli K-12 could be reduced by MnO2 mediated transformation. The results are helpful for understanding the environmental behavior and potential risk of m-AP in natural environment.

中文翻译:

水钠锰矿(δ-MnO2)介导的氧化过程对间氨基苯酚的转化:反应动力学,途径和毒性评估。

间氨基苯酚(m-AP)是一种广泛使用的工业化学品,它随着废物的排放进入水,土壤和沉积物中。发现一种常见的土壤金属氧化物水钠锰矿(δ-MnO2)在酸性条件下以高速率介导m-AP的转化。由于m-AP转化的高度复杂性,因此采用了基于机理的模型来拟合m-AP的转化动力学过程。结果表明,前驱体形成速率限制模型可以描述δ-MnO2对m-AP的转化。δ-MnO2表面上m-AP的氧化转化高度依赖于反应物浓度,pH,温度和其他共溶质。UV-VIS吸光度和质谱分析表明,导致m-AP转化的途径可能是通过偶联反应的聚合。活化能和质谱的结果表明,m-AP自由基很可能通过m-AP芳环中未取代的C2,C4或C6原子之间的共价键结合形成低聚物。此外,转化产物的毒性评估表明,MnO2介导的转化可以降低m-AP对大肠杆菌K-12的毒性。研究结果有助于理解自然环境中m-AP的环境行为和潜在风险。MnO2介导的转化可以减少大肠杆菌K-12。研究结果有助于理解m-AP在自然环境中的环境行为和潜在风险。MnO2介导的转化可以减少大肠杆菌K-12。研究结果有助于理解自然环境中m-AP的环境行为和潜在风险。
更新日期:2019-10-19
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