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Photo-assisted electrochemical production of HClO and Fe2+ as Fenton-like reagents in chloride media for sulfamethoxazole degradation

机译:HCLO和Fe2 +的照片辅助电化学生产作为氯化物介质中的Fenton样试剂,用于磺胺甲恶唑降解

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The photoelectro-Fenton (PEF)-like process based on the replacement of H2O2 by HClO remains quite unexplored. Its ability to mineralize solutions containing 0.208 mM of the antibiotic sulfamethoxazole (SMX), either in 25 mM Na2SO4 + 35 mM NaCl or 45 mM Na2SO4 + 15 mM NaCl media, has been evaluated. The assays were performed in a 3 L pre-pilot flow plant composed of a filter-press FM01-LC reactor, which was equipped with an Ir-Sn-Ru oxide anode and a stainless steel cathode, coupled to an annular photoreactor containing a 160 W UVA lamp. A higher amount of active chlorine (HClO) was produced as the electrolysis was prolonged and the current density was increased. The accumulated HClO concentration dropped down more rapidly at a greater Fe2+ content due to the enhanced oxidant decomposition that yielded center dot OH in the bulk. A continuous production of this radical was ensured from the effective Fe2+ regeneration, being favored by cathodic reduction and photoreduction of dissolved Fe(III) species. The SMX degradation was faster in 25 mM Na2SO4 + 35 mM NaCl mM because of the quicker HClO generation, although the larger proportion of recalcitrant chloro-derivatives and iron-chlorocomplexes decelerated the mineralization process. In 45 mM Na2SO4 + 15 mM NaCl, the best PEF-like treatment was attained at 0.4 mM Fe2+ and 15 mA cm(-2), achieving the complete antibiotic disappearance at 60 min and 59.7% mineralization after 420 min, with an energy consumption of 0.776 kWh (g TOC)(-1). Sixteen intermediates were detected by gas chromatography-mass spectroscopy, ten of which were chlorinated, allowing the proposal of a reaction route for SMX. Since the final solutions did not contain chloro-organics, the partial mineralization was mainly related to the accumulation of refractory non-chlorinated carboxylic acids that could not form photoactive Fe(III)-carboxylate complexes because of the presence of iron-chlorocomplexes.
机译:基于HCLO更换H2O2的光电芬顿(PEF) - 样过程仍然是非常庞大的。已经评估了其含有0.208mm抗生素磺胺甲氧酶(SMX)的溶液的矿化溶液,其在25mM Na 2 SO 4 + 35mM NaCl或45mM Na 2 SO 4 + 15mM NaCl培养基中。该测定在由滤滤网压力机FM01-LC反应器组成的3L预先先导流动设备中进行,其配备有IR-SN-RU氧化物阳极和不锈钢阴极,耦合到含有160的环形光反应器W uva灯。制备较高量的活性氯(HCLO),因为电解延长并且电流密度增加。由于增强的氧化分解,累积的HCLO浓度在更大的Fe2 +含量下更快地降低了氧化剂分解的较大的氧化剂分解。从有效的Fe2 +再生中确保了对该基团的连续产生,通过阴极还原和溶解Fe(III)物种的光电引起的。由于较快的HCLO产生,25mM Na 2 SO 4 + 35mm NaCl Mm的SMX降解在25mM Na 2 SO 4 + 35mm NaCl MM中,尽管氯代氯衍生物和铁 - 氯纤维复合的比例较大,减速了矿化过程。在45mM Na 2 SO 4 + 15mM NaCl中,最佳的PEF样处理在0.4mm FE2 +和15 mA cm(-2)下,在420分钟后在60分钟后实现完全抗生素消失,59.7%的矿化,能耗0.776千瓦时(G TOC)( - 1)。通过气相色谱 - 质谱检测十六个中间体,其中十分之一氯化,允许对SMX进行反应途径的提议。由于最终溶液不含氯有机物,因此部分矿化主要与难治性非氯化羧酸的积累有关,由于存在铁 - 氯复合物,不能形成光活性Fe(III) - 羧酸盐配合物。

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