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铁(Ⅲ)席夫碱配合物的合成及其对新型环境污染物酞酸丁酯的降解性能

Preparation of Fe(Ⅲ) Schiff-base Complex as Catalyst for the Degradation of Emerging Contaminants Dibutyl Phthalate(DBP)

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【作者】 叶夏珺翁乐仪汪雨霏蒋琦沈昊宇胡美琴

【Author】 YE Xiajun;WENG Leyi;WANG Yufei;JIANG Qi;SHEN Haoyu;HU Meiqin;Ningbo Institute of Technology, Zhejiang University;

【通讯作者】 沈昊宇;

【机构】 浙江大学宁波理工学院

【摘要】 通过水杨醛(salicylideimine,SA)与四乙烯五胺(tetraethylenepentamine,TEPA)缩合反应合成了四乙烯五胺水杨醛亚胺席夫碱配体ST [ST=N, N’-tetraethylenepentaminebis(salicylideimine)],进一步与铁(Ⅲ)配位得到双核铁(Ⅲ)配合物[Fe2(ST)(H2O)4]Cl4[简写为Fe2(ST)]。通过元素分析(EA)、红外光谱(FTIR)、紫外可见光谱(UV-Vis)等手段对其进行了表征。以其为催化剂,考察了在双氧水作用下,可见光降解水中新型环境污染物酞酸丁酯(DBP)的性能。结果表明,pH在3.5~8.0范围内,Fe2(ST)的浓度大于5.5 mmol/L,H2O2的浓度大于8.2 mmol/L,10 min内催化体系可以实现对浓度小于20.0 mg/L的DBP 99%以上的降解。监测了加入H2O2前后的反应体系电子光谱随时间的变化,结果表明催化剂的活性位点可能为μ-N桥联的双核Fe(Ⅲ)活性中心,形成了有利于H2O2活化的过渡态。催化体系在循环使用10次后,对DBP的降解率仍可达95%。Fe2(ST)是具有优异潜力的水中酞酸丁酯污染物的绿色催化剂。

【Abstract】 Schiff base ligand(ST = N, N’-tetraethylene pentaminebis(salicylideimine) was prepared by condensation reaction of salicylaldehyde(SA) and tetraethylenepentamine(TEPA), and further coordinated with iron(Ⅲ) via coordination reaction to form a binuclear iron(Ⅲ) complex, [Fe2(ST)(H2 O)4]Cl4(abbreviated as Fe2(ST)). It was characterized by elemental analysis(EA), Fourier transform infrared spectrometer(FTIR), and ultraviolet-visible spectroscopy(UV-vis), etc. It was used as catalyst for the degradation of emerging contaminants, e. g., dibutyl phthalate(DBP) under visible light with hydrogen peroxide solution as oxidant. The results show that at pH 3.5~8.0,with the initial concentration of Fe2(ST) complex larger than 5.5 mmol/L, and that of H2O2 larger than 8.2 mmol/L,the degradation of DBP at initial concentration less than 20.0 mg/L can be reached to almost 99% within 10 minutes. The catalytic reaction system has been monitored by electronic spectrum before or after adding H2O2 at different time intervals. The results show the catalytic activity site may be a μ-N-bridged binuclear Fe(Ⅲ) center and a di-Fe(Ⅲ)-H2O2 transition-state might be formed. The Fe2(ST) can be reused after regeneration for at least 10 times with degradation percentage of DBP over 95%. The Fe2(ST) is a potentially effective and green catalyst for the degradation of DBP.

【基金】 国家自然科学基金(51608479);浙江省自然科学基金(LY14B04003);国家级大学生创新创业训练计划项目(201713022009);浙江省新苗计划项目(2016R401181)
  • 【文献出处】 三峡生态环境监测 ,Ecology and Environmental Monitoring of Three Gorges , 编辑部邮箱 ,2019年01期
  • 【分类号】X703
  • 【被引频次】1
  • 【下载频次】269
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