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Two Advanced Oxidation Pathways of Modified Iron-shavings Participation in Ozonation
Separation and Purification Technology ( IF 8.6 ) Pub Date : 2020-03-10 , DOI: 10.1016/j.seppur.2020.116838
He Wang , Xiaozi Lin , Yuanxing Huang , Weilin Bian , Luming Ma

In this study, the performance of ozonation, catalytic ozonation and activation of molecular oxygen (AMO) process was examined with oxalate as the target refractory organics. Modified iron-shavings was used as catalyst for catalytic ozonation in degradation of oxalate at ambient temperature (25±2℃). Under catalytic ozonation, the removal of oxalate was as high as 90%, which was much better than ozone alone. Initial pH was a key factor affecting the mechanisms of oxalate degradation. In AMO process, with the existence of Fe(II) there occurred an inner-Fenton reaction, hydrogen peroxide(H2O2) was produced at initial pH2.27 and its concentration ranged from 120 to 200 μmol/L. Heterogeneous catalytic ozonation occurred in alkaline solution with hydroxyl radicals (·OH) production, which was indirectly oxidation instead of inner-Fenton reaction. Carbonate would be produced in alkaline solution during catalytic ozonation of oxalate which would in turn inhibit the process. Lepidocrocite(γ-FeOOH) was formed through the dissolved iron ions precipitation and considered as the main component of catalyst, which was confirmed via field emission scanning electron microscope with energy-dispersive spectrometer (SEM-EDS), X-ray powder diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Hydroxyl radicals produced via different mechanisms were detected out by electron paramagnetic resonance (EPR) and were considered as strong oxidant in catalytic ozonation and AMO process.



中文翻译:

改性铁屑参与臭氧化的两种高级氧化途径

在这项研究中,以草酸盐为目标耐火有机物,研究了臭氧化,催化臭氧化和分子氧活化的过程。在环境温度(25±2℃)下,改性铁屑被用作催化臭氧氧化降解草酸盐的催化剂。在催化臭氧化作用下,草酸盐的去除率高达90%,这比单独使用臭氧要好得多。初始pH是影响草酸盐降解机理的关键因素。在AMO过程中,由于Fe(II)的存在,发生了内部Fenton反应,即过氧化氢(H 2 O 2))是在初始pH2.27时产生的,其浓度范围为120至200μmol/ L。在碱性溶液中发生非均相催化臭氧氧化反应,生成羟基自由基(·OH),这是间接氧化而不是内部芬顿反应。在草酸盐的催化臭氧化过程中,将在碱性溶液中生成碳酸盐,这反过来又会抑制该过程。通过溶解的铁离子沉淀形成了锂铁云母(γ-FeOOH),并认为它是催化剂的主要成分,通过场发射扫描电子显微镜和能量分散光谱仪(SEM-EDS),X射线粉末衍射(XRD)证实了)和X射线光电子能谱(XPS)。

更新日期:2020-03-10
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