Degradation of p-Nitrophenol using magnetic Fe0/Fe3O4/Coke composite as a heterogeneous Fenton-like catalyst

Degradation of p-Nitrophenol using magnetic Fe0/Fe3O4/Coke composite as a heterogeneous Fenton-like catalyst
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DOI:
10.1016/j.scitotenv.2016.08.042
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发表时间:
2017-01-01
影响因子:
9.8
通讯作者:
Wei, Xiaobi
Wei, Xiaobi
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Wan, Dong;Li, Wenbing;Wei, Xiaobi

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首次制备了焦炭负载Fe 3 O 4和Fe-0复合物(Fe-0/Fe 3 O 4/Coke),考察了其作为芬顿降解对硝基苯酚(p-NP)的非均相催化剂的性能。采用Box-Behnken四因素设计(BBD)结合响应面法(RSM)考察了Fe-0/Fe 3 O 4/焦炭投加量、反应温度、初始pH和H2 O2浓度对p-NP去除率的影响。使用方差分析(ANOVA)导出显著二次模型(p值< 0.0001,R-2 = 0.9952)。确定最佳条件为13 g/L催化剂,32 ℃,pH 3.1和113 mM H2 O2。在最佳反应条件下,反应120 min,100 mg/L的p-NP转化率达到100%,COD去除率达到81%,与模型预测结果吻合较好。Fe-0/Fe 3 O 4/焦炭的可循环性也进行了研究,在三个连续的运行,其中p-NP降解,性能表现出轻微的差异与第一个氧化循环具有可接受的铁浸出。此外,根据气相色谱-质谱(GC-MS)分析的主要中间产物,提出了基于氢自由基([H])或羟基自由基(中心点OH)机制的p-NP降解途径。(C)© 2016 Elsevier B. V.版权所有。
A Coke supported Fe3O4 and Fe-0 composite (Fe-0/Fe3O4/Coke) was prepared for the first time with the aim of evaluating its ability to be used as heterogeneous catalyst for the Fenton degradation of p-Nitrophenol (p-NP). A four factor Box-Behnken design (BBD) coupled with response surface methodology (RSM) was applied to evaluate the effects of several operating parameters, namely Fe-0/Fe3O4/Coke dosage, reaction temperature, initial pH and H2O2 concentration, on the removal efficiency of p-NP. A significant quadratic model (p-value < 0.0001, R-2 = 0.9952) was derived using analysis of variance (ANOVA). Optimum conditions were determined to be 13 g/L catalyst, 32 degrees C, pH 3.1 and 113 mM H2O2. 100% of p-NP (100 mg/L) conversion and 81% of COD removal were achieved after 120 min of reaction time, respectively, under the optimum conditions, which agreed well with the modeling prediction. The recyclability of Fe-0/Fe3O4/Coke was also investigated after three successive runs, in which p-NP degradation, performances showed a slight difference with the first oxidation cycle with an acceptable iron leaching. Moreover, according to the main intermediate products identified by gas chromatography-mass spectrometry (GC-MS), a possible pathway of p-NP degradation was proposed based on hydrogen radicals ([H]) or hydroxyl radicals (center dot OH) mechanism. (C) 2016 Elsevier B.V. All rights reserved.