Ce-Mn/Al_2O_3-H_2O_2催化氧化皮革废水的研究
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摘要
以浸渍法制备了Ce-Mn/Al_2O_3催化剂,研究该催化剂在H_2O_2非均相类Fenton体系中对皮革废水污染物的催化降解性能.在单因素试验的基础上,以COD去除率为响应值,采用Box-Behnken响应曲面法考察了催化剂投加量、H_2O_2投加量、初始pH、反应时间等4个因素之间的单独作用及交互作用,实验数据用Design-Expert 8.0.6软件进行处理,得到二次响应曲面模型.结果表明,4个独立变量对响应值的影响顺序如下:初始pH>H_2O_2投加量>催化剂投加量>反应时间,数学模型拟合度高(R_(adj)~2=0.9349),利用该模型预测的最大COD去除率为78.86%,最佳反应条件为:催化剂投加量56.63 g·L~(-1),H_2O_2投加量315.15 mg·L~(-1),初始pH3.51,反应时间2 h,经实验验证COD去除率为80.94%,与模型预测值偏差2.08%.
The Ce-Mn/Al_2O_3 was prepared with an impregnation method and was used as catalyst in H_2O_2 heterogeneous Fenton-like system for the degradation of pollutants in tannery wastewater. Based on the single factor tests, the Box-Behnken response surface methodology was utilized to evaluate the simple and combined effects of catalyst dosage, H_2O_2 dosage, initial pH and reaction time on the COD removal efficiency. Data analysis was conducted with Design-Expert 8.0.6, and the quadratic response model was developed. The results show that the significance of influence factors follow the order: initial pH>H_2O_2 dosage>catalyst dosage>reaction time. Furthermore, the model well fits the experimental results(R_(adj)~2=0.9349). From the model, the maximum COD removal efficiency was 78.86%, under the optimized condition with a catalyst dosage at 56.63 g·L~(-1), H_2O_2 dosage at 315.15 mg·L~(-1), initial pH 3.51 and the reaction time of 2 h. The experiment under such condition obtained a COD removal of 80.94%. The experimental value agreed well with the predicted value with 2.08% deviation.
The Ce-Mn/Al_2O_3 was prepared with an impregnation method and was used as catalyst in H_2O_2 heterogeneous Fenton-like system for the degradation of pollutants in tannery wastewater. Based on the single factor tests, the Box-Behnken response surface methodology was utilized to evaluate the simple and combined effects of catalyst dosage, H_2O_2 dosage, initial pH and reaction time on the COD removal efficiency. Data analysis was conducted with Design-Expert 8.0.6, and the quadratic response model was developed. The results show that the significance of influence factors follow the order: initial pH>H_2O_2 dosage>catalyst dosage>reaction time. Furthermore, the model well fits the experimental results(R_(adj)~2=0.9349). From the model, the maximum COD removal efficiency was 78.86%, under the optimized condition with a catalyst dosage at 56.63 g·L~(-1), H_2O_2 dosage at 315.15 mg·L~(-1), initial pH 3.51 and the reaction time of 2 h. The experiment under such condition obtained a COD removal of 80.94%. The experimental value agreed well with the predicted value with 2.08% deviation.
引文
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郑展望, 雷乐成, 张珍, 等. 2004. 非均相UV/Fe-Cu-Mn-Y/H2O2反应催化降解4BS染料废水[J]. 环境科学学报, 24(6): 1032-1038
Elabbas S, Ouazzani N, Mandi L, et al. 2016. Treatment of highly concentrated tannery wastewater using electrocoagulation: Influence of the quality of aluminium used for the electrode[J]. Journal of Hazardous Materials, 319: 69-77
Fan J, Guo Y, Wang J, et al. 2009. Rapid decolorization of azo dye methyl orange in aqueous solution by nanoscale zerovalent iron particles[J]. Journal of Hazardous Materials, 166(2/3): 904-910
Fayazi M, Taher M A, Afzali D, et al. 2016. Enhanced Fenton-like degradation of methylene blue by magnetically activated carbon/hydrogen peroxide with hydroxylamine as Fenton enhancer[J]. Journal of Molecular Liquids, 216: 781-787
高湘, 崔克, 董宏宇, 等. 2017. 好氧接触氧化+Fenton组合工艺处理皮革废水[J]. 环境工程学报, 11(3): 1369-1374
Hou L, Wang L, Royer S, et al. 2016. Ultrasound-assisted heterogeneous Fenton-like degradation of tetracycline over a magnetite catalyst[J]. Journal of Hazardous Materials, 302: 458-467
Huang D, Hu C, Zeng G, et al. 2017. Combination of Fenton processes and biotreatment for wastewater treatment and soil remediation[J]. Science of the Total Environment, 574: 1599-1610
贾永强, 李伟, 贾立庄, 等. 2014. Fenton氧化深度处理高浓度造纸废水的中试实验[J]. 环境工程学报, 8(1): 215-221
李章良, 黄建辉, 郑盛春. 2013. 超声-Fenton联用技术深度处理皮革综合废水生化出水[J]. 环境工程学报, 7(6): 2038-2044
罗钰, 白波, 王洪伦, 等. 2017. Mn@海藻酸微球吸附去除盐酸四环素及其类Fenton再生[J]. 环境科学学报, 37(5): 1732-1741
Rai S K, Konwarh R, Mukherjee A K. 2009. Purification, characterization and biotechnological application of an alkaline β-keratinase produced by Bacillus subtilis RM-01 in solid-state fermentation using chicken-feather as substrate[J]. Biochemical Engineering Journal, 45(3): 218-225
Sharma S, Malaviya P. 2016. Bioremediation of tannery wastewater by chromium resistant novel fungal consortium[J]. Ecological Engineering, 91: 419-425
Song Z, Williams C J, Edyvean R G J. 2004. Treatment of tannery wastewater by chemical coagulation[J]. Desalination, 164(3): 249-259
Wang N, Zheng T, Zhang G, et al. 2016. A review on Fenton-like processes for organic wastewater treatment[J]. Journal of Environmental Chemical Engineering, 4(1): 762-787
Zou X, Zhou T, Mao J, et al. 2014. Synergistic degradation of antibiotic sulfadiazine in a heterogeneous ultrasound-enhanced Fe0/persulfate Fenton-like system[J]. Chemical Engineering Journal, 257: 36-44
王成军, 黄瑞敏, 卿海波, 等. 2008. Fenton试剂法深度处理皮革废水生化出水的研究[J]. 工业用水与废水, 39(2): 49-51
王勇, 李伟光, 宿程远, 等. 2012. 响应曲面法优化均相Fenton深度处理皮革废水[J]. 环境科学学报, 32(10): 2408-2414
肖惠群, 顾早立, 陶智伟, 等. 2015. Fenton氧化法预处理并提高垃圾渗沥液可生化性的研究[J]. 环境科学学报, 35(12): 3937-3942
谢成, 晏波, 韦朝海, 等. 2007. 焦化废水Fenton氧化预处理过程中主要有机污染物的去除[J]. 环境科学学报, 27(7): 1101-1106
张姗姗, 孙正男, 陈海, 等. 2017. Fe3O4/TiO2-H2O2非均相类Fenton体系对3,4-二氯三氟甲苯的降解[J]. 环境科学学报, 37(4): 1374-1380
郑展望, 雷乐成, 张珍, 等. 2004. 非均相UV/Fe-Cu-Mn-Y/H2O2反应催化降解4BS染料废水[J]. 环境科学学报, 24(6): 1032-1038