研究报告

  • 刘萍,王棣,王琳玲,陈静,娄伟,刘平波,吴晓晖.小分子有机醇强化过硫酸盐氧化水中二苯甲酮-3的研究[J].环境科学学报,2021,41(12):4871-4879

  • 小分子有机醇强化过硫酸盐氧化水中二苯甲酮-3的研究
  • Anhydrous alcohols enhanced peroxydisulfate oxidation of Benzophenone-3 in aqueous solution
  • 基金项目:国家重点研发计划项目(No.2016YFC0400704)
  • 作者
  • 单位
  • 刘萍
  • 华中科技大学环境科学与工程学院, 武汉 430074
  • 王棣
  • 华中科技大学环境科学与工程学院, 武汉 430074
  • 王琳玲
  • 华中科技大学环境科学与工程学院, 武汉 430074
  • 陈静
  • 华中科技大学环境科学与工程学院, 武汉 430074
  • 娄伟
  • 湖南省工业固废资源化与安全处置工程技术研究中心(湖南省和清环境科技有限公司), 长沙 410032
  • 刘平波
  • 中国城市建设研究院有限公司, 武汉 430074
  • 吴晓晖
  • 华中科技大学环境科学与工程学院, 武汉 430074
  • 摘要:探究了小分子有机醇对过二硫酸盐(Peroxydisulfate, PDS)氧化降解二苯甲酮-3(Benzophenone-3, BP-3)的强化作用及反应机制.研究结果表明,4种有机醇(甲醇、丙醇、乙二醇和丙三醇)均在一定浓度范围内能有效促进过硫酸盐氧化降解BP-3,BP-3的降解速率随醇类分子碳链长度和羟基数目的增加而增加,增强效果依次为丙三醇>乙二醇>丙醇>甲醇.在低添加量时(21.9~350 μmol·L-1),有机醇的添加增加了BP-3降解速率,但随着醇量的增加呈现出先增大后减小的趋势,例如丙三醇添加量从21.9 μmol·L-1增加到87.6 μmol·L-1,BP-3降解动力学常数从2.91×10-4 s-1提高到3.58×10-4 s-1,增加了0.23倍;但加入过多的醇却抑制了BP-3的降解,例如丙三醇添加量从87.6 μmol·L-1进一步增加到350 μmol·L-1,BP-3降解速率降低29.0%(2.54×10-4 s-1).反应温度也能有效促进醇的强化作用,温度从40 ℃升至60 ℃,添加丙三醇87.6 μmol·L-1,BP-3的降解速率常数从6.84×10-6 s-1提高至6.69×10-4 s-1,提高了96.8倍.小分子有机醇主要是通过与·OH反应产生醇自由基,进一步激活过硫酸盐产生SO4·-,显著增加了SO4·-的产率,从而加速过硫酸盐降解BP-3的效率.
  • Abstract:This paper explored the machanism of peroxydisulfate (PDS) oxidation of benzophenone-3 (BP-3) promoted by small molecule organic alcohols. The results indicated that all four organic alcohols (methanol, propanol, ethylene glycol and glycerol), within a certain concentration range, effectively promoted PDS degradation of BP-3. The enhanced degradation rate of BP-3 varied with the chain length and the number of hydroxyl groups in the alcohols molecules, in the order of glycerol>ethylene glycol>propanol>methanol. At low dosages (21.9~350 μmol·L-1), the addition of organic alcohols increased the degradation rate of BP-3. But further increase of alcohol dosage resulted in a decrease of the degradation rate. Specifically, with the addition of glycerol increased from 21.9 μmol·L-1 to 87.6 μmol·L-1, the degradation kinetic constant of BP-3 increased 0.23 times from 2.91×10-4 s-1 to 3.58×10-4 s-1. However, too much addition of alcohol inhibited the degradation of BP-3. For example, further increased glycerol from 87.6 μmol·L-1 to 350 μmol·L-1, the degradation rate of BP-3 was reduced by 29.0% (2.54×10-4 s-1). The reaction temperature also influenced reaction rate, and when temperature was increased from 40 ℃ to 60 ℃, with 87.6 μmol·L-1 glycerol addition, the degradation rate constant of BP-3 was increased by 96.8 times from 6.84×10-6 s-1 to 6.69× 10-4 s-1. Small molecular organic alcohols mainly generated alcohol free radicals by reacting with ·OH, which further activated persulfate to produce SO4·-, and significantly increased the yield of SO4·-, thereby accelerating the efficiency of the PDS degradation of BP-3.

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