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Selectivity of hydrogen peroxide decomposition towards hydroxyl radicals in catalytic wet peroxide oxidation (CWPO) over Fe/AC catalysts

机译:Fe / AC催化剂上的湿式催化过氧化氧化(CWPO)中过氧化氢分解对羟基的选择性

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Two Fe/AC catalysts prepared with different iron precursors (iron nitrate and iron pentacarbonyl)nand the same AC support have been tested in H2O2 decomposition in presence and absence ofnmethanol, a known strong scavenger of hydroxyl radicals, to investigate the selectivity towardsnzOH formation in this reaction and their behavior in the CWPO of phenol. The catalyst preparednwith iron nitrate, with the most oxidized surface and the highest Fe surface content, seemsnto favor a higher selectivity towards zOH formation in CWPO allowing for complete phenolnconversion and a significant TOC removal, with the highest mineralization degree at 508C andnatmospheric pressure. Fe/AC catalysts were more efficient in the CWPO of phenol than innmethanol presence due to a better use of the oxidant since adsorbed phenol on catalystnsurface minimizes inefficient H2O2 decomposition to H2O and O2(g). The influence of the initialnH2O2 concentration on phenol oxidation with this catalyst was also studied. A theoreticalnstoichiometric amount of H2O2 for complete oxidation of phenol was chosen as the bestnstarting concentration since auto-scavenging reactions can be minimized and it isnsufficient for oxidizing phenol and the aromatic intermediates.
机译:在存在和不存在已知的羟自由基强清除剂-甲醇存在和不存在的情况下,在H2O2分解中测试了使用不同的铁前体(硝酸铁和五羰基铁)和相同的AC载体制备的两种Fe / AC催化剂,以研究在此过程中对nzOH形成的选择性。反应及其在苯酚的CWPO中的行为。用硝酸铁制备的催化剂,具有最大的氧化表面和最高的Fe表面含量,似乎有利于提高CWPO中zOH形成的选择性,从而实现完全的苯酚转化和有效的TOC去除,在508°C和大气压下具有最高的矿化度。 Fe / AC催化剂在苯酚的CWPO中比在无水甲醇中更有效,这是由于氧化剂的更好使用,因为在催化剂表面吸附的苯酚使H2O2分解为H2O和O2(g)的效率降至最低。还研究了初始nH2O2浓度对这种催化剂对苯酚氧化的影响。选择能够完全氧化苯酚的理论化学计算量的H2O2作为最佳起始浓度,因为可以将自清除反应减至最小,并且对于氧化苯酚和芳族中间体并不足够。

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