Preparation of Fe2O3@SCe heterogeneous fenton catalyst and its degradation exothermic performance
YAN Yun-tao, ZHANG Ke, MAO Yan-peng, DONG Yong
National Engineering Laboratory for Reducing Emissions from Coal Combustion, Engineering Research Center of Environmental Thermal Technology of Ministry of Education, Shandong Key Laboratory of Energy Carbon Reduction and Resource Utilization, School of Energy and Power Engineering, Shandong University, Jinan 250061, China
Abstract:Exothermic laws of a heterogeneous Fenton system in the degradation of organic sewage were investigated to facilitate the energy utilization in sewage treatment practices. In this study, semicoke (SCe) was used as the carrier to prepare a novel Fe2O3@SCe composite material, which was then characterized by Brunauer, Emmett, and Teller surface area analysis, Fourier-transform infrared spectroscopy, x-ray diffraction, and scanning electron microscopy. The degradation performance and exothermic laws of the Fe2O3@SCe/H2O2 heterogeneous Fenton system for the treatment of o-phenylenediamine (OPD) organic sewage were studied. The results showed that Fe2O3 was uniformly loaded on the surface of the SCe particles. The Fe2O3@SCe composite material retained its porous form and exhibited strong adsorption capacity and high catalytic activity over a wide pH range (3.1~8.9), an effective broadening of the pH range of the classic homogeneous Fenton reaction. Both the dissolution reactions in Fe2O3@SCe/H2O2 heterogeneous Fenton and the degradation reactions of Fe2O3@SCe/H2O2 and simulated OPD sewage released large amounts of heat. The temperature of the solution reached 7.1℃ higher and was accompanied by a degradation efficiency of 88.2% under the following experimental conditions: [OPD] = 0.04mol/L, pH = 7.8, T0 = 30℃, [H2O2] = 0.25mol/L, [Fe2O3@SCe] = 533g/L, and t = 180min. The concentration of H2O2 was found to be the dominant factor affecting exothermic heat release during the heterogeneous Fenton reaction.
刘文正,赵帅,柴茂林,等.采用辉光放电等离子体的烟气处理技术研究[J].中国环境科学, 2017,37(8):2905-2914. Liu W Z, Zhao S, Chai M L, et al. Technology of flue gas treatment with glow discharge plasma[J]. China Environmental Science, 2017, 37(8):2905-2914.
[2]
郑逸武,段钰锋,汤红健,等.燃煤烟气污染物控制装置协同脱汞特性研究[J].中国环境科学, 2018,38(3):862-870. Zheng Y W, Duan Y F, Tang H J, et al. Characteristics of the existing air pollutant control devices on Hg synergistic removal in a coal-fired power plant[J]. China Environmental Science, 2018,38(3):862-870.
[3]
武娟妮,程亮,逯元堂,等.散煤采暖清洁化替代方式的生命周期清单分析[J].中国环境科学, 2018,38(4):1570-1578. Wu J N, Cheng L, Lu Y T, et al. Life cycle inventory analysis of clean alternatives to scattered coal heating. China Environmental Science, 2018,38(4):1570-1578.
[4]
王春兰,许诚,徐钢,等.京津冀地区天然气和热泵替代燃煤供暖研究[J].中国环境科学, 2017,37(11):4363-4370. Wang C L, Xu C, Xu G, et al. Studies on replacing coal with natural gas and heat pump for heating in Jing-Jin-Ji region[J]. China Environmental Science, 2017,37(11):4363-4370.
[5]
王智伟,李扬,孙海洋,等.直接式污水源热泵蒸发器、冷凝器污垢生长测试研究[J].西安建筑科技大学学报, 2014,46(4):567-571. Wang Z W, Li Y, Sun H Y. Test and research on the fouling in condenser and evaporator of direct sewage source heat pump system[J]. Xi'an Univ. of Arch. & Tech.:Natural Science Edition, 2014,(4):567-571
[6]
吴月,孙宇维,王岽,等.曝气及外加H2O2强化电芬顿法处理石化反渗透浓水[J].化工进展, 2017,36(9):3523-3530. Wu Y, Sun Y Y, Wang D, et al. Enhanced treatment of petrochemical reverse osmosis concentrate by an electro-Fenton process with dosing H2O2 and aeration[J]. Chemical Industry and Engineering Progress, 2017,36(9):3523-3530.
[7]
方嘉声,于光认,陈晓春,等.石墨烯掺杂分子筛负载氧化铁芬顿催化降解苯酚影响因素的研究[J].环境科学学报, 2015,35(11):3529-3537. Fang J S, Yu G R, Chen X C, et al. The influence factors on the Fenton catalytic degradation of phenol using iron-loaded graphene modified molecular sieve catalyst[J]. Acta Scientiae Circumstantiae, 2015, 35(11):3529-3537.
[8]
王列,姚玉元,孙利杰,等.活性炭纤维耦合柠檬酸铁在中性pH条件下活化双氧水降解染料[J].化学学报, 2013,71(12):1633-1638. Wang L, Yao Y Y, Sun L J, et al. Activation of hydrogen peroxide by activated carbon fibers coupled with Fe (Ⅲ)-Citrate for Degradation of Dyes at Neutral pH[J]. Acta Chimica Sinica, 2013,71(12):1633-1638.
[9]
包木太,王娜,陈庆国,等. Fenton法的氧化机理及在废水处理中的应用进展[J].化工进展, 2008,27(5):660-665. Bao M T, Wang N, Chen Q G, et al. Oxidation mechanism and application progress of Fenton process in wastewater treatment[J]. Chemical Industry and Engineering Progress, 2008,27(5):660-665.
[10]
徐丹,张丽丽,柳丽芬,等.Cu-Al2O3中骨架铜类芬顿催化去除水中有机污染物[J].环境科学, 2017,38(3):1044-1060. Xu D, Zhang L L, Liu L F. Fenton-like catalytic removal of organic pollutants in water by framework Cu in Cu-Al2O[J]. Environmental Science, 2017,38(3):1044-1060.
[11]
蒋胜韬,祝建中,管玉江,等.非均相类Fenton法降解硝基苯化工废水的效能及其机制[J].化工学报, 2014,65(4):1487-1494. Jiang S T, Zhu J Z, Guan Y J, et al. Performance of heterogeneous Fenton-like system for degradation of nitrobenzene-containing wastewater[J]. CIESC Journal, 2014,65(4):1488-1494.
[12]
朱峥嵘,王明新,张金永,等. Fe (VI)/CaO2双氧化体系降解水环境中的DMP[J].中国环境科学, 2019,39(7):2838-2846. Zhu Z R, Wang M X, Zhang J Y, et al. Degradation performance of dimethyl phthalate from aqueous environment by dual oxidant of ferrate/calcium peroxide[J]. China Environmental Science, 2019,39(7):2838-2846.
[13]
杨涛,李国朝,杨期勇,等.Fenton试剂协同预涂动态膜处理乳化油废水[J].化工进展, 2013,32(4):942-945. Yang T, Li G C, Yang Q Y, et al. A coupling process of pre-coating dynamic membrane with Fenton reagent for treatment of oily wastewater[J]. Chemical Industry and Engineering Progree, 2013, 32(4):942-945.
[14]
杨波,张永丽.非均相芬顿体系协同去除复合双污染物:化学转化, pH影响和机理分析[J].化学学报, 2019,77(10):1017-1023. Yang B, Zhang Y L. Synergistic removal of Co-contamination by heterogeneous fenton system:Chemical conversion, pH effect and mechanism analysis[J]. Acta Chimica Sinica, 2019,77(10):1017-1023.
[15]
黄丹维,何佳,谷亚威,等.球磨微米硫化零价铁活化双氧水降解有机污染物的研究[J].化学学报, 2017,75(9):866-872. Huang D W, He J, Gu Y W, et al. Mechanochemically sulfidated zero valent iron as an efficient fenton-like catalyst for degradation of organic contaminants[J]. Acta Chim. Sinica, 2017,75(9):866-872.
[16]
李午阳,徐乐瑾.废水中有机污染物降解机理的研究方法[J].化学学报, 2019,77(8):705-716. Li W Y, Xu L J. Research methods for the degradation mechanism of organic pollutants in wastewater[J]. Acta Chim. Sinica, 2019,77(8):705-716.
[17]
邓景衡,文湘华,李佳喜.碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝[J].环境科学学报, 2014,34(6):1436-1442. Deng J H, Wen X H, Li J X. Degradation of methylene blue by heterogeneous Fenton-like reaction using Fe3O4/carbon nanotube composites[J]. Acta Scientiae Circumstantiae, 2014,34(6):1436-1442.
[18]
于晓丹,林鑫辰,冯威,等.Fe3O4/TiO2@生物碳骨架复合材料的一步法制备及UV-Fenton催化性能[J].高等学校化学学报, 2018, 39(11):2500-2506. Yu X D, Lin X C, Feng W, et al. One-step Preparation and UV-Fenton Properties of Fe3O4/TiO2@Bio-carbon Composities†[J]. Chemical Journal of Chinese Universities, 2018,39(11):2500-2506.
[19]
严梅,张青,谢慧芳,等.纳米Fe3O4负载聚苯胺对染料的协同催化降解[J].中国环境科学, 2017,37(4):1394-1400. Yan M, Zhang Q, Xie H F, et al. Load of PANI on nano-Fe3O4 and synergy catalytic degradation of dyes[J]. China Environmental Science, 2017,37(4):1394-1400.
[20]
Yan Y T, Mao Y P, Dong Y, et al. Exothermic laws applicable to the degradation of o-phenylenediamine in wastewater via a Fe3+/H2O2 homogeneous quasi-Fenton system[J]. RSC ADVANCES, 2019, 9(45):26283-26290.
[21]
Mishra A. K., Ramaprabhu S. Magnetite decorated multiwalled carbon nanotube basedSupercapacitor for arsenic removal and desalination of seawater[J]. Journal of physicalchemistry C, 2010, 114(6):2583-2590.
[22]
王炫,李焕焕,张乾,等.蛋白土-Fe2O3非均相Fenton催化剂高效降解罗丹明B染料废水[J].化工进展, 2017,36(8):3116-3124. Wang X, Li H H, Zhang Q, et al. Research on opal-Fe2O3 as a heterogeneous Fenton catalyst for degrading the Rhodamine B dye wastewater[J]. Chemical Industry and Engineering Progress, 2017, 36(8):3116-3124.
[23]
孙浩,吴娟,马东,等.钒酸铁类Fenton催化剂的制备及性能研究[J].中国环境科学, 2015,35(6):1734-1739. Sun H, Wu J, Ma D, et al. Preparation of iron (III) vanadate Fenton-like catalyst and its catalytic performance[J]. China Environmental Science, 2015,35(6):1734-1739.
[24]
魏晓币,王光华,李文兵,等.磁性Fe3O4/改性焦炭的制备及其降解性能[J].化工进展, 2017,36(7):2577-2583. Wei X B, Wang G H, Li W B, et al. Preparation and degradation properties of magnetic Fe3O4/modified coke[J]. Chemical Industry and Engineering Progress, 2017,36(7):2577-2583.
[25]
张巨擘,孙晓晗,高桥娇,等.可再生Fe3O4/CuFeS2/生物质复合降解柱对有机染料的处理性能.高等学校化学学报, 2019,40(3):425-430. Zhang J, Sun X, Gao Q, et al. Degradation of organic dyes over regenerative Fe3O4/CuFeS2/biomass composite column[J]. Chemical Journal of Chinese Universities, 2019,40(3):425-430.
[26]
吕来,胡春.多相芬顿催化水处理技术与原理[J].化学进展, 2017,29(9):981-999. Lü L, Hu C. Heterogeneous fenton catalytic water treatment technology and mechanism[J]. Progress in Chemistry, 2017,29(9):981-999.
[27]
王炜亮,王玉番,卢少勇,等.US/UV-Fenton体系处理高浓度罗丹明B特性研究[J].中国环境科学, 2016,36(8):2329-2336. Wang W L, Wang Y F, Lu S Y, et al. Characteristic studies on treatment of high concentration rhodamine B with US/UV-Fenton system[J]. China Environmental Science, 2016,36(8):2329-2336.
[28]
Maz C, Li J S, Xing S T. Facile cyclohexane-mediated hydrothermal synthesis of modified δ-MnO2 with enhanced fenton-like catalytic activity[J]. Chemical Journal of Chinese Universities, 2017,38(4):636-641.
[29]
Qian Y J, Zhang J, Zhang Y L, et al. Degradation of 2,4 dichlorophenol by nanoscale calcium peroxide:Implication for groundwater remediation[J]. Separation and Purification Technology, 2016,166:222-229.
[30]
曾萍,刘诗月,张俊珂,等.芬顿法深度处理生物处理排水中的四环素抗性基因[J].中国环境科学, 2017,37(9):3315-3323. Zeng P, Liu S Y, Zhang J K, et al. advanced Fenton oxidation treatment of tetracycline resistance genes in effluent discharged from biological wastewater treatment[J]. China Environmental Science, 2017,37(9):3315-3323.
[31]
张武,纪妍妍,彭涵,等.FeY型分子筛的高效制备及非均相Fenton催化降解性能.高等学校化学学报, 2018,39(9):1985-1992. Zhang W, Ji Y Y, Peng H, et al. High efficiency synthesis of FeY type zeolite and its heterogeneous fenton catalytic degradation[J]. Chemical Journal of Chinese Universities, 2018,39(9):1985-1992.
[32]
董家麟,付双,周昊,等.纳米过氧化钙对地下水中硝基苯的类-Fenton降解效果[J].中国环境科学, 2019,39(11):4730-4736. Dong J, Fu S, Zhou H, et al. Effect of nano calcium peroxide on the fenton-like degradation of nitrobenzene in groundwater[J]. China Environmental Science, 2019,39(11):4730-4736.