Cooperation of Fe(II) and peroxymonosulfate for enhancement of sulfamethoxazole photodegradation: mechanism study and toxicity elimination.
Cooperation of Fe(II) and peroxymonosulfate for enhancement of sulfamethoxazole photodegradation: mechanism study and toxicity elimination.
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Fe(II) 与过一硫酸盐协同增强磺胺甲恶唑光降解：机理研究和毒性消除
作者：
本研究旨在系统地考察Fe(II)光辅助过一硫酸盐(PMS)活化去除水溶液中新出现的污染物磺胺甲恶唑(SMX)的潜力。采用高效液相色谱法测定SMX的残留量。监测了SMX降解过程中Fe(II)([Fe(II)])的浓度。Fe(II)和PMS之间的协同作用使SMX的光降解速度加快；Fe(II)和PMS之间的摩尔比相对较低或较高时，由于自由基或清除作用不足，导致SMX的去除效率较低。与[Fe(II)]0Δ ： 0.5 mM或[pMS]0 ： 0 0.2 5 mm的反应在前5分钟检测到[Fe(II)]≥0与1.6≤1的固定反应比.采用UVA+Fe(II)+PMS工艺处理SMX时，最佳pH值为6.0左右。通过UPLC/ESI-MS分析检测到6个转化产物，其中4个为新报道。根据异恶唑-环平衡和Beer-Lambert定律计算了中间体的浓度。降解过程中总有机碳的减少主要归因于苯环的损失、N-S裂解和异恶唑的开环。根据猝灭试验确定了活性物种OH·和SO4·−的贡献。该处理方法消除了SMX对轮虫的急性毒性，证明该工艺对SMX的处理是有效的，对环境是安全的。本研究首次系统地揭示了UV/Fe(II)/过一硫酸盐去除磺胺甲恶唑的潜力、机理和风险。
This study aims at systematically examining the potential of removing the emerging pollutant sulfamethoxazole (SMX) from aqueous solution under photo-assisted peroxymonosulfate (PMS) activation by Fe(ii). The residual SMX was determined by HPLC analysis. The concentration of Fe(ii) ([Fe(ii)]) was monitored during SMX degradation. Fe(ii) and PMS cooperated with each other for faster SMX photodegradation; a relatively lower or higher molar ratio between Fe(ii) and PMS led to lower SMX removal efficiency due to the insufficient radicals or scavenging effect. A fixed reaction ratio of [Fe(ii)]Δ : [PMS]0 with 1.6 : 1 at the first 5 min was detected for reactions with [Fe(ii)]0 ≥ 0.5 mM or [PMS]0 ≤ 0.25 mM. The pH level of around 6.0 was recommended for optimal SMX removal under the treatment process UVA + Fe(ii) + PMS. Six transformation products were detected through UPLC/ESI-MS analysis, and four of the proposed intermediates were newly reported. Concentrations of the intermediates were proposed based on the isoxazole-ring balance and the Beer–Lambert law. Total Organic Carbon (TOC) reduction was mainly attributed to the loss of benzene ring, N–S cleavage, and isoxazole ring opening during SMX degradation. The contributions of reactive species OH˙ and SO4˙− were determined based on quench tests. The acute toxicity of SMX to the rotifers was eliminated after the proposed treatment, demonstrating that the process was effective for SMX treatment and safe to the environment. For the first time, this study systematically revealed the potential, the mechanism and the risk of removing sulfamethoxazole by UV/Fe(II)/peroxymonosulfate.
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