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首页> 外文期刊>RSC Advances >Generation of reactive cobalt oxo oxamate radical species for biomimetic oxidation of contaminants
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Generation of reactive cobalt oxo oxamate radical species for biomimetic oxidation of contaminants

机译：产生反应性钴的氧化酯的污染物仿染色氧化物种

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摘要

The non-heme oxamate anionic cobalt(III) complexes [CoIII(opbaX)](-) (opbaX = 4-X-ophenylenebis( oxamate), X = H, NO2, CH3) with different substituents were synthesized and applied to targeted micropollutant degradation. Typical radical scavengers (isopropanol and chlorine anions) have no negative effect on the catalytic oxidation of substrates, and no DMPO-cOH or DMPO-cOOH (DMPO = 5,5-dimethyl-pyrroline-oxide) signal was detected by electron paramagnetic resonance spin-trap technique in [CoIII(opbaX)](-)/H2O2 system, suggesting that the non-hydroxyl radical biomimetic catalytic mechanism was dominant in the oxidation process. The results of high-definition ESI-MS pronounced the presence of cobalt-oxo intermediates which played a key role in the catalytic oxidation of substrates. Furthermore, density functional theory calculations were used to evaluate the viability of such cobaltoxo species and it demonstrated an optimizing electromer with a formulation of [CoIV] Oc](-) or [(CoOH)-O-III] c. The calculations explained that the catalytic activity of [CoIII(opbaX)](-) was significantly enhanced by introducing an electron-withdrawing substituent which could change the coordination environment of cobalt to generate more electron-deficient cobalt-oxo species with stronger oxidizing power. This paper made a progress in verifying bio-mimic high oxidation state species and applied it to water purification, which provided deep insight into the properties of transition-metal centers in aqueous catalysis.
机译：合成非血红素氧基甲酸钴（III）络合物[COIII（OPBAX）]（ - ）（OPBAX = 4- X-二聚基亚（OPAMATE），X = H，NO2，NO2，CH3）并施加到靶向微污染物上降解。典型的自由基清除剂（异丙醇和氯阴离子）对底物的催化氧化没有负面影响，并且通过电子顺磁共振旋转检测DMPO-COH或DMPO-COOH（DMPO = 5,5-二甲基 - 吡咯烷酰基氧化物）信号-Trap技术在[COIII（OPBAX）]（ - ）/ H 2 O 2系统中，表明非羟基自由基仿催化机制在氧化过程中显着。高清ESI-MS的结果发出了存在的钴 - 氧代中间体，其在底物的催化氧化中发挥了关键作用。此外，使用密度函数理论计算来评估这种钴藻物种的可行性，并表现出具有[COIV] OC]（ - ）或[（COOH）-O-III] C的配方的优化电力。该计算说明通过引入电子抽出的取代基来显着提高[CoIII（OPBAX）]（ - ）的催化活性，这可以改变钴的配位环境以产生更强的氧化能力的更高的电子缺乏钴 - 氧代物种。本文在验证生物模拟高氧化态物种并将其应用于净水中进行了进展，这提供了深入了解过渡金属中心在水性催化中的性质。

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  • 来源
    《RSC Advances》 |2017年第68期|共9页
  • 作者

    Li Nan; Zheng Yun; Jiang Xuemei; Zhang Ran; Chen Wenxing;

  • 作者单位

    Zhejiang Sci Tech Univ Natl Engn Lab Text Fiber Mat &

    Proc Technol Zheji Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Sci Tech Univ Natl Engn Lab Text Fiber Mat &

    Proc Technol Zheji Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Sci Tech Univ Natl Engn Lab Text Fiber Mat &

    Proc Technol Zheji Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Sci Tech Univ Natl Engn Lab Text Fiber Mat &

    Proc Technol Zheji Hangzhou 310018 Zhejiang Peoples R China;

    Zhejiang Sci Tech Univ Natl Engn Lab Text Fiber Mat &

    Proc Technol Zheji Hangzhou 310018 Zhejiang Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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