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Oxidative degradation of p-chloroaniline by copper oxidate activated persulfate

机译:氧化铜活化过硫酸盐氧化降解对氯苯胺

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Oxidation of p-chloroaniline (PCA) by persulfate (PS) performed with a novel supported copper oxidate catalyst in an aqueous solution at ambient temperature (i.e. 20 °C) was investigated in this study. This study focused mainly on determining the proportions of heterogeneous catalysis in the copper oxidate/PS combined system. There existed a more remarkable effect on the degradation of PCA in the copper oxidate/PS combined system than in the Cu~(2+)/PS or only PS system. The effects of copper oxidate dosage, persulfate concentration, and initial solution pH on the oxidation of PCA were also evaluated. Higher copper oxidate dosage and persulfate concentration resulted in higher PCA degrading rates, the optimal initial pH was determined as 7.0. Moreover, the change in the degradation of PCA by pH was also investigated in terms of the contribution of dissolved copper ion in leaching solution. We inferred that homogeneous catalysis was of increasing importance and the copper ion dissolved from the copper oxidate was regarded as the key factor activating the persulfate under acidic conditions (pH 3.0), heterogeneous catalysis played the main role in the oxidation of PCA at pH 5-7. However, both heterogeneous catalysis and base-activated persulfate contributed to the degradation of PCA under alkaline conditions (pH 11). In addition, the radical mechanism was studied and three radical scavengers (phenol, methanol (MA) and Tert-butanol (TBA)) were used to determine the kind of major active areas taking part in the PCA degradation at pH 7.
机译:在这项研究中,研究了在水溶液中,使用新型的负载型氧化铜催化剂在水溶液中用过硫酸盐(PS)氧化对氯苯胺(PCA)的方法。这项研究主要集中于确定氧化铜/ PS组合系统中非均相催化的比例。与Cu〜(2 +)/ PS或仅PS体系相比,氧化铜/ PS组合体系对PCA的降解作用更为显着。还评估了氧化铜用量,过硫酸盐浓度和初始溶液pH值对PCA氧化的影响。较高的氧化铜剂量和过硫酸盐浓度导致较高的PCA降解速率,最佳初始pH确定为7.0。此外,还根据浸出液中溶解的铜离子的贡献,研究了pH引起的PCA降解的变化。我们推断,均相催化的重要性日益增加,从氧化铜中溶解的铜离子被认为是在酸性条件下(pH 3.0)激活过硫酸盐的关键因素,非均相催化在pH 5的PCA氧化中起主要作用。 7然而,在碱性条件下(pH 11),多相催化和碱活化的过硫酸盐均会导致PCA降解。此外,研究了自由基机理,并使用三种自由基清除剂(苯酚,甲醇(MA)和叔丁醇(TBA))确定了在pH 7下参与PCA降解的主要活性区域的类型。

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