锰铁复合氧化物催化臭氧化脱色木醋液
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摘要
用共沉淀法制备了锰铁复合氧化物催化剂。利用X射线粉末衍射(XRD),比表面积分析仪(BET)及扫描电子显微镜(SEM)对催化剂进行表征,并测试催化剂臭氧化降解脱色木醋液性能。结果表明,制备的锰铁复合氧化物催化剂具有与层状MnO_2相同的晶体结构;随着铁含量的增加,其形貌由仙人球状转变为片状,比表面积也由26.4 m~2/g增大到74.1 m~2/g。锰铁复合氧化物催化臭氧化相对于单一使用臭氧表现出更好的脱色效果,且含铁比例越大效果越好;催化剂使用量的增加以及提高pH值都有利于木醋液降解脱色。
Mn-Fe binary oxides were prepared by co-precipitation method and tested in the catalytic ozonation of wood vinegar. The catalysts were characterized by X-ray diffraction(XRD), specific surface area analyzer(BET) and scanning electron microscope(SEM). The results showed that Mn-Fe oxides have the crystal structure same as that of layered MnO_2. With the increase of iron content in Mn-Fe oxides, the morphology transformed from prickly pear-like shape to flake and the specific surface area significantly increased from 26.4 to 74.1 m~2/g. By the use of Mn-Fe oxide catalysts, ozonation was enhanced for the decolorization of wood vinegar. High catalytic activity was observed over the Mn-Fe oxides with high Fe/Mn molar ratio. In addition, it was found that high pH value of solution favored the decolorization of wood vinegarr.
Mn-Fe binary oxides were prepared by co-precipitation method and tested in the catalytic ozonation of wood vinegar. The catalysts were characterized by X-ray diffraction(XRD), specific surface area analyzer(BET) and scanning electron microscope(SEM). The results showed that Mn-Fe oxides have the crystal structure same as that of layered MnO_2. With the increase of iron content in Mn-Fe oxides, the morphology transformed from prickly pear-like shape to flake and the specific surface area significantly increased from 26.4 to 74.1 m~2/g. By the use of Mn-Fe oxide catalysts, ozonation was enhanced for the decolorization of wood vinegar. High catalytic activity was observed over the Mn-Fe oxides with high Fe/Mn molar ratio. In addition, it was found that high pH value of solution favored the decolorization of wood vinegarr.
引文
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[2] Kanetake T,Kanetake A.Removal of Phenol from Pyroligneous Acid:JP10088145 [P].1998-04-07.
[3] Yatagai M,Nishimoto M,Hori K,et al.Termiticidal Activity of Wood Vinegar,Its Components and Their Homologues[J].J Wood Sci,2002,48(4):338-342.
[4] Wu Q,Zhang S,Hou B,et al.Study on the Preparation of Wood Vinegar from Biomass Residues by Carbonization Process [J].Bioresour Technol,2015,179:98-103.
[5] Xu Y M,Liu Q,Zhang Q M,et al.Research Progress on Application of CMA Environmentally Friendly Deicer [J].Chem World,2010,51(7):435-437.(许英梅,刘倩,张秋民,等.CMA类环保型融雪剂的应用研究进展[ J].化学世界,2010,51(7):435-437.)
[6] Xu Y M,Zhang Q M,Jiang H M,et al.Preparation of Environment Friendly Calcium-magnesium Acetate Deicers from Pyroligneous Liquid [J].J Dalian Univ Technol,2007,47(4):494-496.(许英梅,张秋民,姜慧明,等.由木醋液制醋酸钙镁盐类环保型融雪剂研究[J] 大连理工大学学报,2007,47(4):494-496.)
[7] Li G,He J,Wang D,et al.Optimization and Interpretation of O3 and O3/H2O2 Oxidation Processes to Pretreat Hydrocortisone Pharmaceutical Wastewater[J].Environ Technol,2015,36(5-8):1 026-1 034.
[8] Hostachy J C,Lenon G,Pisicchio J L,et al.Reduction of Pulp and Paper Mill Pollution by Ozone Treament [J].Water Sci Technol,1997,35(2):261-268.
[9] Wang B,Yuan Z,Li Y T,et al.Treatment of Drilling Wastewater by Mn3O4 Catalytic Ozonation[J].Chin J Environ Eng,2015,9(7):3 319-3 324.(王兵,袁增,李永涛,等.Mn3O4 催化臭氧化处理钻井废水[J].环境工程学报,2015,9(7):3 319-3 324.)
[10] Qi L L,Yao J,You H,et al.Oxidation Products and Degradation Pathways of 4-Chlorophenol by Catalytic Ozonation with MnOx/γ-Al2O3/TiO2 as Catalyst in Aqueous Solution [J].J Environ Sci Health A,2014,49(3):327-337.
[11] Faria P C C,Monteiro D C M,Orfao J J M,et al.Cerium,Manganese and Cobalt Oxides as Catalysts for the Ozonation of Selected Organic Compounds [J].Chemosphere,2009,74(6):818-824.
[12] Cui H J,Huang H Z,Yuan B,et al.Decolorization of RhB Dye by Manganese Oxides:Effect of Crystal Type and Solution pH [J].Geochem Trans,2015,16(1):10.
[13] Abdelli G,Leitner N K V.Oxidation of Cyanuric Acid in Aqueous Solution by Catalytic Ozonation [J].Ozone Sci Eng,2015,38(3):233-241.
[14] He H,Wu D,Lv Y,et al.Enhanced Mineralization of Aqueous Reactive Black 5 by Catalytic Ozonation in the Presence of Modified GAC [J].Desalin Water Treat,2016,57:14 997-15 006.
[15] Wei L Y,Ma J Y,Liu Y J.Pretreatment of Refinery Wastewater by Heterogeneous Catalytic Ozonation [J].Petrochem Technol,2013,42(2):210-215.(魏令勇,马静园,刘月佳.臭氧多相催化氧化预处理石油炼制污水[J].石油化工,2013,42(2):210-215.)
[16] Qian F Y,Wang F F,Liu X M,et al.Catalytic Ozonation Based on Carbon Materials for Removing Dissolved Organic Compounds from Water:A Review[J].Chem Ind Eng Prog,2015,34(6):1 755-1 761.(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):1 755-1 761.)
[17] Jiang S J,Liu Z Y.The Meaning of UV254 as an Organic Matter Monitoring Parameter in Water Supply & Wastewater Treatment [J].J Chongqing Jianzhu Univ,2002,24(2):61-65.(蒋绍阶,刘宗源.UV254 作为水处理中有机物控制指标的意义[J].重庆建筑大学学报,2002,24(2):61-65.)