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首页> 外文期刊>Chemical engineering journal >Catalytic oxidative degradation of bisphenoi A using an ultrasonic-assisted tourmaline-based system: Influence factors and mechanism study
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Catalytic oxidative degradation of bisphenoi A using an ultrasonic-assisted tourmaline-based system: Influence factors and mechanism study

机译:超声辅助电气石基体系催化双酚A的催化氧化降解:影响因素及机理研究

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摘要

Tourmaline was utilized as a heterogeneous catalyst for the oxidation of bisphenoi A (BPA) with syner-getic H2O2-catalytic ability and ultrasonic irradiation. Higher tourmaline concentration, an appropriate H2O2 dose and a lower pH favored BPA depletion. The removal of 5.0 mg L~(-1) BPA reached 98.4% at 120 min under the following optimized reaction conditions: sonication (40 kHz, 500 W), tourmaline concentration 5.0 g L~(-1) H2O2 50 mM and pH 2.0. This high BPA removal could be caused by coordinating heterogeneous and homogeneous processes, based on the observed iron leaching and H2O2 conversion data at different pHs. A retarded first-order kinetic model was employed to describe BPA degradation. The strong inhibition of BPA removal by radical scavengers indicated that the attack of hydroxyl radicals was mainly responsible for BPA removal. In view of the X-ray photoelectron spectroscopy (XPS) results during the reaction, a possible mechanism involving accelerated transfer in the Fe(III)/Fe(II) cycle on the tourmaline surface was proposed. Moreover, eight intermediates were evidenced by GC-MS and LC-MS/MS analyses, and a reaction pathway was also proposed, including the processes of hydroxylation, oxidative skeletal rearrangement, demethylation and dehydration.
机译:电气石被用作具有协同H2O2催化能力和超声辐射的双酚A(BPA)氧化的非均相催化剂。较高的电气石浓度,适当的H2O2剂量和较低的pH值有利于BPA的消耗。在以下优化的反应条件下,于120 min时,去除5.0 mg L〜(-1)BPA的去除率达到98.4%:超声处理(40 kHz,500 W),电气石浓度5.0 g L〜(-1)H2O2 50 mM和pH 2.0 。基于观察到的铁浸出和不同pH值下的H2O2转化数据,这种高BPA去除可能是由于协调异质过程和均质过程引起的。延迟的一级动力学模型被用来描述BPA降解。自由基清除剂对BPA去除的强烈抑制作用表明,羟基自由基的攻击主要是BPA去除的原因。鉴于反应过程中的X射线光电子能谱(XPS)结果,提出了一种可能的机制,涉及在电气石表面上的Fe(III)/ Fe(II)循环中加速转移。此外,通过GC-MS和LC-MS / MS分析证实了八种中间体,并且还提出了反应途径,包括羟基化,氧化性骨架重排,脱甲基和脱水的过程。

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