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首页> 外文期刊>Frontiers in Chemistry >CWPO Degradation of Methyl Orange at Circumneutral pH: Multi-Response Statistical Optimization, Main Intermediates and by-Products
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CWPO Degradation of Methyl Orange at Circumneutral pH: Multi-Response Statistical Optimization, Main Intermediates and by-Products

机译：在环境pH值下CWPO降解甲基橙：多响应统计优化，主要中间体和副产物

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The catalytic wet peroxide oxidation (CWPO) of the industrial azo-dye methyl orange (MO) activated by an Al/Fe-pillared clay catalyst was optimized by the Response-Surface Methodology (RSM). Three sequential sets of factorial 2k central composite experiments were required for the full optimization of the process; catalyst loading and stoichiometric dose of hydrogen peroxide were the experimental factors studied through different times of reaction by means of all, Dissolved Organic Carbon (DOC) removal, Total Nitrogen (TN) removal, reacted fraction of hydrogen peroxide and decolourization as experimental responses to be maximized. The resulting single-response RSM optimums were combined in a multi-response Desirability function ruling out the differential effect of adsorption on the catalyst’s surface by defining all responses per gram of clay catalyst. Former two statistical sets of experiments (DOE-1 and DOE-2) showed the CWPO degradation of MO to get favored at increasing both catalyst loading and time of reaction (up to 180 min). Afterwards, third final design of experiments (DOE-3) displayed 75 % of DOC removal, 78 % of TN removal, 97 % of reacted H2O2 and 95 % of decolourization by using a catalyst loading of 5.0 g/L of Al/Fe-PILC together with just 50 % of the stoichiometric amount of H2O2. The multi-response optimum conditions based on the Desirability function showed excellent fitting explaining at least 99.3 % of the optimal overall responses at 95 % confidence. A further analysis revealed that no one of the non-controllable variables under real conditions of industrial wastewater treatment (covariates): starting total organic carbon (TOC) (2.0 – 20 mg/L), temperature (5.0 – 25 °C) or circumneutral pH (6.0 – 9.0), exhibited statistically significant effect (P–values 0.05), suggesting the system to be almost insensitive against them within studied range of close to ambient conditions in the tropic. Finally, HPLC/PDA and GC/FID measurements identified phenol, Cyclohexa-2,5-diene-1,4-dione, Phenylamine, N-methylaniline and N,N-dimethylaniline in very low concentrations as main intermediates in the CWPO degradation of MO, which nevertheless disappeared over 90 min of treatment. Meanwhile, 4-aminobenzenesulfonic and oxalic acids were recorded as unique by-products at final time of reaction, but both fairly less toxic than the starting azo-dye.
机译：通过响应表面法（RSM）优化了铝/铁立柱粘土催化剂活化的工业偶氮染料甲基橙（MO）的催化湿式过氧化物氧化（CWPO）。完整优化工艺需要三个顺序的阶乘2k中央复合实验。过氧化氢的催化剂负载和化学计量量是通过不同反应时间研究的实验因素，包括溶解有机碳（DOC）去除，总氮（TN）去除，过氧化氢的反应分数和脱色作为实验响应。最大化。最终得到的单响应RSM最优值与多响应合意函数结合在一起，通过定义每克粘土催化剂的所有响应，排除了催化剂表面吸附的不同影响。前两组统计实验（DOE-1和DOE-2）显示，MO的CWPO降解在增加催化剂负载量和反应时间（长达180分钟）时得到了促进。之后，实验的第三最终设计（DOE-3）通过使用5.0 g / L的Al / Fe-催化剂负载量，去除了75％的DOC，78％的TN，97％的反应过的H2O2和95％的脱色。 PILC以及仅化学计算量的H2O2的50％。基于Desirability函数的多响应最佳条件显示出极好的拟合，可以解释在95％置信度下至少99.3％的最佳总体响应。进一步的分析表明，在工业废水处理的真实条件下，没有任何一个不可控变量（协变量）：起始总有机碳（TOC）（2.0 – 20 mg / L），温度（5.0 – 25°C）或周围温度pH（6.0 – 9.0）表现出统计学上的显着影响（P-值> 0.05），表明该系统在热带地区接近环境条件的研究范围内几乎对它们不敏感。最后，HPLC / PDA和GC / FID测量确定了非常低浓度的苯酚，环己-2,5-二烯-1,4-二酮，苯胺，N-甲基苯胺和N，N-二甲基苯胺是CWPO降解的主要中间体。 MO，但在治疗90分钟后消失。同时，4-氨基苯磺酸和草酸在反应的最后时间被记录为独特的副产物，但是它们的毒性都比起始的偶氮染料低。

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