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在瀑布式反应器中使用基于羟基/硫酸根自由基的技术对苯胺进行矿化处理。

Mineralization of aniline using hydroxyl/sulfate radical-based technology in a waterfall reactor.

作者信息

Durán A, Monteagudo J M, San Martín I, Amunategui F J, Patterson D A

机构信息

Department of Chemical Engineering, Grupo IMAES, Escuela Técnica Superior de Ingenieros Industriales, Instituto de Investigaciones Energéticas y Aplicaciones Industriales (INEI), Universidad de Castilla-La Mancha, Avda. Camilo José Cela 3, 13071, Ciudad Real, Spain.

Department of Chemical Engineering, Grupo IMAES, Escuela Técnica Superior de Ingenieros Industriales, Instituto de Investigaciones Energéticas y Aplicaciones Industriales (INEI), Universidad de Castilla-La Mancha, Avda. Camilo José Cela 3, 13071, Ciudad Real, Spain.

出版信息

Chemosphere. 2017 Nov;186:177-184. doi: 10.1016/j.chemosphere.2017.07.148. Epub 2017 Jul 29.

Abstract

The aim of this work is to study the applicability of a UV/HO process intensified with persulfate (PS) as a source of SO radicals to efficiently mineralize a synthetic effluent containing aniline in a glass reactor arranged in a cascade configuration. pH conditions were studied and the concentration of PS was optimized. The synergism for aniline mineralization between the UV/HO process and the combined UV/HO/PS process was quantified in 10.1%. Aniline degradation reached 100% under the UV/H2O2/PS process after 20 min. Its mineralization is favored under acidic conditions and with the presence of persulfate (optimal conditions: 49% in 90 min; pH = 4; [PS] = 250 ppm). On the contrary, the worst conditions were found at pH = 11, since hydrogen peroxide decomposes and carbonates were formed increasing the scavenging effect. The different mechanisms involved (formulated from intermediates identified by mass spectrometry) confirm these results. Aniline was found to follow a degradation pathway where phenol is the main intermediate. The presence of sulfate radicals increases phenol degradation rate leading to a higher mineralization extent. Benzoquinone was identified as the main aromatic oxidation product of phenol, whereas succinic, 4-oxo-pentanoic, fumaric and oxalic acids were detected as aliphatic oxidation products for both UV/H2O2 and UV/H2O2/PS oxidation processes.

摘要

这项工作的目的是研究以过硫酸盐(PS)作为SO自由基源强化的UV/HO工艺在级联配置的玻璃反应器中对含苯胺的合成废水进行有效矿化的适用性。研究了pH条件并优化了PS的浓度。UV/HO工艺与UV/HO/PS组合工艺之间苯胺矿化的协同作用定量为10.1%。在UV/H2O2/PS工艺下,20分钟后苯胺降解率达到100%。在酸性条件下且存在过硫酸盐时有利于其矿化(最佳条件:90分钟内矿化率为49%;pH = 4;[PS] = 250 ppm)。相反,在pH = 11时发现条件最差,因为过氧化氢分解并形成碳酸盐,增加了清除效应。所涉及的不同机理(由质谱鉴定的中间体推导得出)证实了这些结果。发现苯胺遵循以苯酚为主要中间体的降解途径。硫酸根自由基的存在提高了苯酚的降解速率,导致更高的矿化程度。苯醌被确定为苯酚的主要芳香族氧化产物,而琥珀酸、4-氧代戊酸、富马酸和草酸被检测为UV/H2O2和UV/H2O2/PS氧化过程的脂肪族氧化产物。

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