高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (7): 1582-1590.doi: 10.7503/cjcu20200143

• 物理化学 • 上一篇    下一篇

纤维负载炭黑金属酞菁轴向配合物仿酶高效催化降解水体中有机污染物

夏云,吕汪洋*(),陈文兴*(),李楠   

  1. 浙江理工大学纺织纤维材料与加工技术国家地方联合工程实验室, 杭州 310018
  • 收稿日期:2020-03-16 出版日期:2020-07-10 发布日期:2020-05-11
  • 通讯作者: 吕汪洋,陈文兴 E-mail:luwy@zstu.edu.cn;wxchen@zstu.edu.cn
  • 基金资助:
    国家自然科学基金(51703201)

Fiber Supported Carbon Black Metal Phthalocyanine Axial Complex to Mimic Enzyme for Highly Efficient Catalytic Degradation of Organic Pollutant in Water

XIA Yun,Lü Wangyang*(),CHEN Wenxing*(),LI Nan   

  1. National Engineering Laboratory for Textile Fiber Materials & Processing Technology, Zhejiang Sci-Tech University, Hangzhou 310018, China
  • Received:2020-03-16 Online:2020-07-10 Published:2020-05-11
  • Contact: Wangyang Lü,Wenxing CHEN E-mail:luwy@zstu.edu.cn;wxchen@zstu.edu.cn
  • Supported by:
    † National Natural Science Foundation of China(51703201)

摘要:

天然血红素基过氧化氢酶具有高选择催化性, 但易失活变性. 为提高其活性和稳定性, 以性能稳定的十六氯铁酞菁(FePcCl16)为活性中心, 四氨基吡啶为配体, 炭黑(CB)为载体, 合成了仿酶催化剂炭黑十六氯铁酞菁轴向配合物(FePcCl16-Py-CB); 通过热黏合法将其负载于低熔点皮芯聚酯纤维(LMPET)上, 生成易与水体分离的纤维负载型仿酶催化剂FePcCl16-Py-CB@LMPET, 并以H2O2为氧化剂, 地赛米松(DXMS)为底物, 构筑仿酶催化体系. 研究了该催化体系在温和条件下的催化性能及循环使用性能, 探讨了催化体系的催化机理及DXMS的降解历程. 结果表明, 异裂H2O2产生的高价铁氧[Fe(Ⅳ)=O]为催化体系中的主要活性物种, 体系呈现出优异的催化性能和稳定性能. 该催化体系在120 min内降解的最终产物均为小分子酸.

关键词: 低熔点皮芯聚酯纤维, 炭黑, 金属酞菁, 仿酶催化剂, 有机污染物

Abstract:

Natural heme catalase has high selective catalysis, but it is easy to deactivate. The enzyme-like catalyst carbon black iron hexadecachlorophthalocyanine axial complex(FePcCl16-Py-CB)was synthesized for improving the activity and stability of enzyme. In the catalyst, FePcCl16 with stable performance worked as active site, tetraminopyridine was introduced as ligand, carbon back was employed as carrier. Fiber-supported enzyme mimicking catalyst FePcCl16-Py-CB@LMPET which was easy to separate with water was prepared by FePcCl16-Py-CB loaded on low melting point sheath-core polyester fibers(LMPET) via thermal bonding. The enzyme-like catalytic system was designed based on FePcCl16-Py-CB@LMPET as catalyst, H2O2 as oxidant, DXMS as substrate to investigate the catalytic activity and the recycle performance, to explore the catalytic mechanism and the degradation process of DXMS. The results showed that high valent iron oxo[Fe(Ⅳ)=O] produced by heterolytic cleavage of H2O2 was the main active species, thus the system exhibited excellent catalytic activity and stable performance under mild condition. The final degradation products of the catalytic system were all small molecular acids within 120 min. The construction of the enzyme-like catalytic system provides a new idea for wastewater treatment.

Key words: Low melting point sheath-core polyester fiber, Carbon black, Metal phthalocyanine, Enzyme-like catalyst, Organic pollutant

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