PREPARATION OF Fe/Mn-PAC CATALYSTS AND DEGRADATION OF REACTIVE BRILLIANT BLUE KN-R BY CATALYTIC OZONATION
-
摘要: 为获得高效去除活性艳蓝的方法,采用浸渍煅烧法制备了Fe/Mn-PAC催化剂,对催化剂的表面形态和结构进行表征,研究了不同因素对KN-R降解效果的影响,以及催化剂的重复利用性和稳定性。结果表明:Fe/Mn-PAC催化剂表面粗糙,具有较多的微孔结构,催化剂表面的金属氧化物为致密的地衣状结构,有利于提升催化剂的催化性能。在催化剂投加量为400 mg/L,初始pH为7.5,Fe/Mn进料比为1∶1及负载量为4%时,Fe/Mn-PAC表现出最佳的催化KN-R降解的反应活性,45 min内KN-R去除率高达90%以上;经过5次回收利用,去除率仍可达到84.7%。研究结果证明了Fe/Mn-PAC催化剂具有优异的催化能力和出色的结构稳定性,为实现印染废水中活性艳蓝KN-R的有效去除提供了技术支持。Abstract: Typical dyestuffs, such as KN-R in printing and dyeing wastewater were difficult to be effectively removed by traditional biochemical treatment technology, due to their biological toxicity and chemical stability, which seriously polluted the water environment. To obtain an efficient KN-R removal approach, Fe/Mn-PAC catalyst was prepared by impregnation calcination. The surface morphology and structure of the catalysts were characterized, and the effects of different factors on the degradation of KN-R were also investigated. Meanwhile, the reusability and stability of the catalysts were studied. It was demonstrated that the Fe/Mn-PAC catalyst had a rough surface with more microporous structures, and the metal oxides on the catalyst surface were dense lichen-like structures, which were conducive to enhancing the catalytic performance. At a catalyst dosage of 400 mg/L, an initial pH of 7.5, an Fe/Mn feed ratio of 1∶1 and a loading amount of 4%, Fe/Mn-PAC showed the best catalytic activity for KN-R degradation, with over 90% of KN-R removed within 45 min. After five recycling cycles, the KN-R removal rate was still 84.7%. The above results demonstrated that the synthesized Fe/Mn-PAC catalyst possessed excellent catalytic capabilities and structural stability, and provided technical support to realize the effective removal of KN-R from printing and dyeing wastewater.
-
[1] BUYUKADA M. Removal of yellow F3R, di maria brilliant blue and reactive brilliant red M-3BE from aqueous solutions by a rapid and efficient ultrasound-assisted process with a novel biosorbent of cottonseed cake: statistical modeling, kinetic and thermodynamic studies[J]. Arabian Journal for Science & Engineering, 2015, 40(8): 2153-2168. [2] ROSA J M, FILETI A M F, TAMBOURGI E B, et al. Dyeing of cotton with reactive dyestuffs: the continuous reuse of textile wastewater effluent treated by Ultraviolet/Hydrogen peroxide homogeneous photocatalysis[J]. Journal of Cleaner Production, 2015, 90: 60-65. [3] WANG S M, GUAN Y, WANG L P, et al. Fabrication of a novel bifunctional material of BiOI/Ag3VO4 with high adsorption-photocatalysis for efficient treatment of dye wastewater[J]. Applied Catalysis B: Environmental, 2015, 168/169: 448-457. [4] ZHANG S C, LU X J. Treatment of wastewater containing Reactive Brilliant Blue KN-R using TiO2/BC composite as heterogeneous photocatalyst and adsorbent[J]. Chemosphere, 2018, 206: 777-783. [5] LI X L, LI X M, YANG W J, et al. Preparation of 3D PbO2 nanospheres@SnO2 nanowires/Ti electrode and its application in methyl orange degradation[J]. Electrochimica Acta, 2014, 146: 15-22. [6] BALAPURE K, JAIN K, BHATT N, et al. Exploring bioremediation strategies to enhance the mineralization of textile industrial wastewater through sequential anaerobic-microaerophilic process[J]. International Biodeterioration & Biodegradation, 2016, 106: 97-105. [7] 马珍珍. GN-NiO复合物在染料废水臭氧化处理中的应用[D]. 郑州:河南大学, 2016. [8] MUNTER R. Advanced oxidation processes: current status and prospects[J]. Cheminform, 2001, 50(2): 59-80. [9] WANG J L, LOU Y Y, XU C, et al. Magnetic lanthanide oxide catalysts: an application and comparison in the heterogeneous catalytic ozonation of diethyl phthalate in aqueous solution[J]. Separation & Purification Technology, 2016, 159: 57-67. [10] 钱飞跃, 王翻翻, 刘小朋, 等. 碳质材料催化臭氧氧化去除水中溶解性有机物的研究进展[J]. 化工进展, 2015, 34(6): 1755-1761. [11] FARIA P, ORFAO J, PEREIRA M. Mineralisation of coloured aqueous solutions by ozonation in the presence of activated carbon[J]. Water Research, 2005, 39(8): 1461-1470. [12] LIU P, HE H P, WEI G L, et al. Effect of Mn substitution on the promoted formaldehyde oxidation over spinel ferrite: catalyst characterization, performance and reaction mechanism[J]. Applied Catalysis B: Environmental, 2016, 182(31): 476-484. [13] LIANG X L, LIU P, HE H P, et al. The variation of cationic microstructure in Mn-doped spinel ferrite during calcination and its effect on formaldehyde catalytic oxidation[J]. Journal of Hazardous Materials, 2016, 306: 305-312. [14] 王维业. 非均相臭氧催化氧化系统研究及其对印染废水的深度处理[D]. 哈尔滨:哈尔滨工业大学, 2016. [15] 刘卫华, 季民, 张昕, 等 催化臭氧氧化去除垃圾渗滤液中难降解有机物的研究[J]. 环境化学, 2007, 26(1): 58-61. [16] YUAN L, SHEN J M, YAN P W, et al. Catalytic ozonation of 4-chloronitrobenzene by goethite and Fe2+-modified goethite with low defects: a comparative study[J]. Journal of Hazardous Materials, 2019, 365: 744-750. [17] LU X H, ZHANG Q Y, YANG W Q, et al. Catalytic ozonation of 2,4-dichlorophenoxyacetic acid over novel Fe-Ni/AC[J]. RSC Advances, 2015, 5(14): 10537-10545. [18] LING W C, QIANG Z M, SHI Y W, et al. Fe(Ⅲ)-loaded activated carbon as catalyst to improve omethoate degradation by ozone in water[J]. Journal of Molecular Catalysis A-Chemical, 2011, 342/343: 23-29. [19] HE H P, WU D L, LV Y P, et al. Enhanced mineralization of aqueous Reactive Black 5 by catalytic ozonation in the presence of modified GAC[J]. Desalination and Water Treatment, 2016, 57(32): 14997-15006. [20] WANG X R, YANG W Z, JI Y, et al. Heterogeneous Fenton-like degradation of methyl blue using MCM-41-Fe/Al supported Mn oxides[J]. RSC Advances, 2016, 6(31): 26155-26162. [21] SUN H, SUN M, ZHANG Y B, et al. Catalytic ozonation of reactive red X-3B in aqueous solution under low pressure: decolorization and OH center dot generation[J]. Frontiers of Environmental Science & Engineering, 2015, 9(4): 591-595. [22] LIN F W, WANG Z H, SHAO J M, et al. Catalyst tolerance to SO2 and water vapor of Mn based bimetallic oxides for NO deep oxidation by ozone[J]. RSC Advances, 2017, 7(40): 25132-25143. [23] GOGOLEV A V, SHILOV V P. Interaction of ozone with variable-valence metal ions in concentrated silicate solutions[J]. Russian Journal of General Chemistry, 2014, 84(8): 1468-1471. [24] DONG S. Research on the heterogeneous catalytic ozonation for the treatment of printing and dyeing wastewater[J]. Industrial Water Treatment, 2013, 33(4): 58-60. [25] OH B S, SONG S J, LEE E T, et al. Catalyzed ozonation process with GAC and metal doped-GAC for removing organic pollutants[J]. Water Science and Technology, 2004, 49(4): 45-49. [26] ZHAO L, MA J, SUN Z Z, et al. Mechanism of influence of initial pH on the degradation of nitrobenzene in aqueous solution by ceramic honeycomb catalytic ozonation[J]. Environmental Science & Technology, 2008, 42(11): 4002-4007. [27] DAI Q Z, WANG J, YU J Y, et al. Catalytic ozonation for the degradation of acetylsalicylic acid in aqueous solution by magnetic CeO2 nanometer catalyst particles[J]. Applied Catalysis B Environmental, 2014, 144(2): 686-693. [28] ZHAO L, SUN Z Z, MA J. Novel relationship between hydroxyl radical initiation and surface group of ceramic honeycomb supported metals for the catalytic ozonation of nitrobenzene in aqueous solution[J]. Environmental Science & Technology, 2009, 43(11): 4157-4163. [29] BAI Z Y, YANG Q, WANG J L. Fe3O4/multi-walled carbon nanotubes as an efficient catalyst for catalytic ozonation of p-hydroxybenzoic acid[J]. International Journal of Environmental Science & Technology, 2016, 13(2): 483-492. [30] LI Y, ZHAO Q H, GE Y H, et al. Catalytic ozonation of salicylic acid in aqueous solutions by metal oxide supported catalysts[J]. Journal of Chemical Engineering of Chinese Universities, 2016, 30(2): 446-453. [31] TANG S F, YUAN D L, ZHANG Q, et al. Fe-Mn bi-metallic oxides loaded on granular activated carbon to enhance dye removal by catalytic ozonation[J]. Environmental Science and Pollution Research, 2016, 23(18): 18800-18808. [32] 王欣奕. 铁锰氧化物负载的活性炭催化臭氧去除亚甲基蓝的效能研究[D]. 哈尔滨:哈尔滨工业大学, 2021.
点击查看大图
计量
- 文章访问数: 212
- HTML全文浏览量: 40
- PDF下载量: 18
- 被引次数: 0