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首页> 外文期刊>Catalysis science & technology >Rapid degradation of oxidation resistant nitrophenols by TAML activator and H2O2
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Rapid degradation of oxidation resistant nitrophenols by TAML activator and H2O2

机译：TAML激活剂和H2O2快速降解抗氧化硝基苯酚

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Nitrophenols (NPs) are widely prevalent recalcitrant anthropogenic pollutants. TAML activators in conjunction with peroxides have proven to be effective in the remediation of myriad organic pollutants. In the present study, we have discovered that one of the most reactive TAML activators [Fe{4,5-Cl2C6H3-1,2-(NCOCMc(2)NCO)(2)CF2}(OH2)](-) (1) catalyses the oxidative degradation by H2O2 of mono-and dinitrophenols (including all US-EPA classified priority pollutants) under ambient conditions at pH 8 which is close to pH of environmental waters. Individual nitrophenols as well as mixtures thereof undergo fast decontamination (reaction time <= 45 min) resulting in deep oxidation producing HCO2- and minerals, CO, CO2, NO2-, and NO3- (up to 99% of N and 70% of C). The remarkable efficacy of the 1/H2O2-mediated decontamination process is matched by complete elimination of the toxicity of the nitrophenols (Microtox (R) assays). Detailed mechanistic studies of the catalyzed oxidation revealed a strong substrate inhibition of the catalytic activity for some nitrophenols, the strongest being observed for 4-nitrophenol. DFT calculations suggest that the inhibition is likely due to reversible binding of nitrophenolate anions to the iron(III) center of the resting state of the 1 catalyst, which compromises its reactivity toward H2O2.
机译：硝基苯酚（NPS）是广泛普遍的顽固性人为污染物。 TAML活化剂与过氧化物结合使用已被证明有效地修复了无数有机污染物。在本研究中，我们发现最具反应性的TAML激活剂之一[Fe {4,5-CL2C6H3-1,2-（NCOCMC（2）NCO（2）NCO）（2）CF2}（OH2）（OH2）]（ - ）（1）（1）（1）（1 ）在pH 8处的环境条件下，H2O2催化H2O2的单硝基苯酚（包括所有US-EPA分类优先污染物）的氧化降解（包括所有US-EPA分类优先污染物）。单个硝基苯酚以及其混合物经历快速净化（反应时间<= 45分钟），导致深层氧化产生HCO2-和矿物质，CO，CO2，NO2-，NO2-和NO3-（最多99％的N和70％的C ）。通过完全消除硝基苯酚（Microtox（r）测定）的毒性，1/H2O2介导的去污过程的显着疗效与之相匹配。催化氧化的详细机械研究表明，对某些硝基苯酚对催化活性有很强的底物抑制，这是4硝基苯酚的最强。 DFT计算表明，抑制作用可能是由于1催化剂静息态的硝基苯甲酸离阴离子的可逆结合，这损害了其对H2O2的反应性。

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