生物相容性pH下铁络合物催化有机污染物的光催化氧化:以O2为主要氧化剂进行类芬顿反应

Xi Chen, Wanhong Ma, Jing Li, Zhaohui Wang, Chungcheng Chen, Hongwei Ji, Jincai Zhao
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引用次数: 42

摘要

研究了一种红色铁(II) 4,4 ' -二羧基-2,2 ' -联吡啶配合物([FeII(dcbpy)3])作为一种特殊的芬顿催化剂,在可见光照射下,能够在生物相容的pH值下激活更多的分子O2来矿化水中的有机污染物。该催化剂具有较高的转化率(368 ~ 2000),可有效降解8种典型的有机污染物。配体dcbpy灵活的双功能配位模式(N供体为亚铁离子,O供体为铁离子)应该负责在这种中性pH条件下保持铁(II/III)的催化作用,而dcbpy中的4,4 ' -羧基被其他基团如醚、醇、硝基或甲基取代导致几乎完全失去催化稳定性。更重要的是,本文所设计的[FeII(dcbpy)3]催化剂能够显著改变h2o2在一般Fenton反应中作为主氧化剂的传统作用,使O2分子在Fenton反应中成为主氧化剂。
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Photocatalytic Oxidation of Organic Pollutants Catalyzed by an Iron Complex at Biocompatible pH Values: Using O2 as Main Oxidant in a Fenton-like Reaction
A red iron(II) 4,4′-dicarboxy-2,2′-bipyridine complex ([FeII(dcbpy)3]) was investigated as an extraordinary Fenton catalyst capable of activating much more molecular O2 to mineralize organic pollutants in water at biocompatible pH values under visible irradiation. Eight representative organic pollutants were effectively degraded in the presence of this catalyst with high turnover number (368−2000). The flexible bifunctional coordination mode (N donor for ferrous ion and O donor for ferric form) devoted by the ligand dcbpy should be responsible for the preservation of iron(II/III) catalysis in such a neutral pH condition, whereas any substitution of the 4,4′-carboxylic groups in dcbpy by other groups such as ether, alcohol, nitroyl, or methyl groups resulted in nearly total loss of catalytic stability. More important, the present [FeII(dcbpy)3] catalyst can dramatically change the traditional role ofH2O2 as main oxidant in the general Fenton reaction and make molecular O2 become the main oxidant in the min...
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