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铁基MOFs非均相催化Fenton体系降解苯酚研究

Iron-based metal organic frameworks as heterogeneous Fenton catalysts for phenol degradation

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【作者】 高聪全燮

【Author】 Cong Gao;Xie Quan;Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education),School of Environmental Science and Technology,Dalian University of Technology;

【机构】 大连理工大学环境学院

【摘要】 非均相Fenton技术是污水处理及环境修复的有效方法,但目前非均相催化剂催化活性较低限制其发展,开发高活性非均相Fenton催化剂对其应用及水污染处理发展是非常有意义的。本研究中将MIL-88B(Fe)应用到Fenton技术中,通过XRD、SEM、IR等表征表明采用水热法成功制备具有良好晶体结构及形貌的MIL-88B(Fe)。以苯酚作为目标污染物,考察了H2O2投加量,催化剂投加量及初始pH对苯酚降解效果的影响并确定苯酚降解过程中起主导作用的自由基。结果表明,对于浓度为50 ppm的苯酚溶液,0.15 g/L MIL-100(Fe),15 m M H2O2在pH=4条件下30min内可以完全降解,苯酚降解效率随着pH升高呈现降低趋势,过量或少量H2O2及催化剂会抑制苯酚降解。MIL-88B(Fe)重复使用3次,其催化活性不发生明显变化。EPR表征表明MIL-88B(Fe)催化非均相Fenton体系中主要存在羟基自由基,羟基自由基猝灭剂实验证明·OH对苯酚降解起主导作用。对比常见非均相Fenton催化剂如α-Fe OOH及Fe3O4,结果显示Fe-MIL-88B催化活性高1-3个数量级,综上表明MIL-88B(Fe)是高催化活性及稳定性的新型非均相Fenton催化剂。

【Abstract】 Heterogeneous Fenton is an attractive technology in environmental remediation,however,the low activity of catalysts have limited their further application.In this work,MIL-88B(Fe) was applied in heterogeneous Fenton reaction for phenol degradation.XRD,SEM,IR and BET were used to characterize the as-prepared MIL-88B(Fe).The effects of dosages of H2O2 and catalysts and initial pH value were evaluated.50 ppm phenol was completely removed by 0.15 g/L MIL-88B(Fe) and 15 m M H2O2 in 30 min at pH=4.The phenol removal decreased with increasing pH value,and inhibited with higher or lower dosages of H2O2 and MIL-88B(Fe).EPR and radical scavenger tests showed ·OH was generated and played a key role in phenol degradation in MIL-88B(Fe) catalyzed Fenton reaction.In addition,MIL-88B(Fe) showed good stability(reused for 3 times without evident activity loss) and 1-3 orders higher catalytic activity than some traditional heterogeneous Fenton catalysts(Fe3O4,α-FeOOH).

  • 【会议录名称】 中国化学会第30届学术年会摘要集-第二十六分会:环境化学
  • 【会议名称】中国化学会第30届学术年会-第二十六分会:环境化学
  • 【会议时间】2016-07-01
  • 【会议地点】中国辽宁大连
  • 【分类号】X703;O643.3
  • 【主办单位】中国化学会
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