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首页> 外文期刊>Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications >Oxidative removal of 4-nitrophenol using activated carbon fiber and hydrogen peroxide to enhance reactivity of metallophthalocyanine
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Oxidative removal of 4-nitrophenol using activated carbon fiber and hydrogen peroxide to enhance reactivity of metallophthalocyanine

机译：使用活性炭纤维和过氧化氢氧化去除4-硝基苯酚以增强金属酞菁的反应性

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摘要

We have developed a novel heterogeneous metallophthalocyanine catalyst, Co-TDTAPc-ACF, by immobilizing cobalt tetra(2,4-dichloro-1,3,5-triazine)aminophthalocyanine (Co-TDTAPc) on activated carbon fiber (ACF) covalently. The oxidative removal of 4-nitrophenol (4-NP) in the Co-TDTAPc-ACF/ H2O2 system, based on phase transfer catalytic oxidation, was investigated in aqueous solution by ultra-performance liquid chromatography (UPLC). The results indicated that 4-NP could be removed efficiently by catalytic oxidation in the presence of Co-TDTAPc-ACF and H2O2. In addition, the removal of total organic carbon of 4-NP accounted for about 90% in 300 min of reaction. Gas chromatography/mass spectrometry (GC-MS) analysis showed that the residue products were mainly small molecular compounds such as maleic acid and succinic acid, etc. This system exhibited high catalytic activity across a wide pH and temperature range. Importantly, compared with homogeneous Co-TDTAPc used alone, the introduction of ACF contributed specifically to the activity enhancement of Co-TDTAPc. Controlled experiments showed that the presence of 2-propanol, as hydroxyl radicals scavenger, has little influence on 4-NP oxidation. The further result of electron paramagnetic resonance (EPR) spin-trap experiments indicated that free radicals did not dominate the reaction in our system. This paper discusses a possible catalytic oxidation mechanism of the Co-TDTAPc-ACF/H2O2 system. Repetitive tests showed that Co-TDTAPc-ACF can maintain high catalytic activity over several cycles, and it has a better regeneration capability under mild conditions. We conclude that phase transfer catalytic oxidation has proven itself to be a feasible approach which may be potentially applied to the elimination of widely existing pollutants.
机译：我们通过将钴四（2,4-二氯-1,3,5-三嗪）氨基酞菁钴（Co-TDTAPc）共价固定在活性炭纤维（ACF）上，开发了一种新型的非均相金属酞菁催化剂Co-TDTAPc-ACF。通过超高效液相色谱法（UPLC）研究了相转移催化氧化在Co-TDTAPc-ACF / H2O2系统中对4-硝基苯酚（4-NP）的氧化去除。结果表明，在Co-TDTAPc-ACF和H2O2存在下，催化氧化可有效去除4-NP。此外，在300分钟的反应中，除去4-NP的总有机碳约占90％。气相色谱/质谱（GC-MS）分析表明，残留产物主要为小分子化合物，例如马来酸和琥珀酸等。该系统在较宽的pH和温度范围内均具有较高的催化活性。重要的是，与单独使用均质Co-TDTAPc相比，ACF的引入特别有助于Co-TDTAPc的活性增强。对照实验表明，作为羟基清除剂的2-丙醇的存在对4-NP氧化的影响很小。电子顺磁共振（EPR）自旋捕集实验的进一步结果表明，自由基在我们的系统中并未控制反应。本文讨论了Co-TDTAPc-ACF / H2O2系统可能的催化氧化机理。重复测试表明，Co-TDTAPc-ACF可以在多个循环中保持较高的催化活性，并且在温和条件下具有更好的再生能力。我们得出的结论是，相转移催化氧化已被证明是一种可行的方法，可以潜在地应用于消除广泛存在的污染物。

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