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采用高温回流法将石墨烯( gh)掺杂于Al?MCM?41介孔分子筛中,通过浸渍法制备了石墨烯改性Al?MCM?41介孔分子筛负载铁芬顿催化剂( gh?Al?MCM?41?Fe),利用比表面仪、扫描电子显微镜?X射线能谱( SEM?EDX )对催化剂进行了表征,考察了不同 pH 条件下该催化剂对苯酚的催化降解效能。结果表明, gh?Al?MCM?41?Fe催化剂具有介孔结构,表明颗粒分布均匀,石墨烯的掺杂减小了颗粒粒径,与多种催化剂(非介孔Al2O3?CuAl2O4、介孔Al2O3?Cu、介孔Al2O3?Fe、介孔Al?MCM?41?Fe)相比,gh?Al?MCM?41?Fe具有最高的苯酚催化降解效能,反应符合一级反应特征,石墨烯的掺杂能明显提高苯酚降解率和COD去除率,减少铁的溶出,拓宽pH范围,当pH值为3—5,反应90 min,COD去除率达到60%以上。

Graphene ( gh) modified mesoporous molecular sieves Al?MCM?41 were synthesized via a high temperature reflow method. Then gh?Al?MCM?41?Fe catalyst was prepared by a impregnation method. The catalyst was characterized by surface analyzer, scanning electron microscopy?energy dispersive X?ray spectrometry ( SEM?EDX) . Fenton catalytic degradation efficiency of phenol under different pH conditions was evaluated. The results showed that gh?Al?MCM?41?Fe possessed mesoporous structure and the particles distributed homogenously. The doped graphene reduced particle size. Compared with various catalysts ( non-mesoporous Al2 O3?CuAl2 O4 , mesoporous Al2 O3?Cu, mesoporous Al2 O3?Fe, mesoporous Al?MCM?41?Fe ) , gh?Al?MCM?41?Fe had the highest catalytic degradation capacity for phenol. The reaction process complied with the first?order kinetics model. The doping of graphene increased the degradation rate of phenol and the removal rate of COD, reduced the iron dissolution and expanded the pH range of the degradation reaction. When pH value was 3—5, the removal rate of COD reached more than 60% after 90 min reaction.

参考文献

[1] 宋瀚文,王东红,徐雄,王海亮,陈锡超,罗茜,王子健,杜迎欣.我国24个典型饮用水源地中14种酚类化合物浓度分布特征[J].环境科学学报,2014(02):355-362.
[2] Juergen Poerschmann;Ulf Trommler .Pathways of advanced oxidation of phenol by Fenton's reagent—Identification of oxidative coupling intermediates by extractive acetylation[J].Journal of chromatography, A: Including electrophoresis and other separation methods,2009(29):5570-5579.
[3] 李海松,闫阳,买文宁,姚萌.铁碳微电解-H2O2耦合联用的类Fenton法处理制浆造纸废水[J].环境化学,2013(12):2302-2306.
[4] 徐小妹,潘顺龙,李健生,孙秀云,沈锦优,韩卫清,王连军.多孔载体负载型Fenton催化剂降解酚类污染物的研究进展[J].化工进展,2014(06):1465-1474.
[5] 陈伟,毕程,李婷婷,郭晶.酞菁锌改性介孔分子筛催化降解孔雀石绿[J].环境化学,2012(07):1043-1048.
[6] Yuhan Ling;Mingce Long;Peidong Hu;Ya Chen;Juwei Huang .Magnetically separable core-shell structural γ-Fe_2O_3@Cu/Al-MCM-41 nanocomposite and its performance in heterogeneous Fenton catalysis[J].Journal of hazardous materials,2014(Jan.15):195-202.
[7] K. Chakarova;G. Petrova;M. Dimitrov .Coordination state of Cu~+ ions in Cu-[Al]MCM-41[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2011(1/2):186-194.
[8] Luan Z H;Cheng C F;Zhou W Z et al.Mesopore molecular sieve MCM-41 containing framework aluminum[J].The Journal of Physical Chemistry,1995,99(3):1018-1024.
[9] ANH LE-TUAN PHAM;CHANGHA LEE;FIONA M. DOYLE .A Silica-Supported Iron Oxide Catalyst Capable of Activating Hydrogen Peroxide at Neutral pH Values[J].Environmental Science & Technology: ES&T,2009(23):8930-8935.
[10] Bautista, P.;Mohedano, A.F.;Casas, J.A.;Zazo, J.A.;Rodriguez, J.J. .Highly stable Fe/γ-Al2O3 catalyst for catalytic wet peroxide oxidation[J].Journal of Chemical Technology & Biotechnology,2011(4):497-504.
[11] Geim A K .Graphene:Status and prospects[J].SCIENCE,2009,324(5934):1530-1534.
[12] C. N. R. Rao;A. K. Sood;K. S. Subrahmanyam .Graphene: The New Two-Dimensional Nanomaterial[J].Angewandte Chemie,2009(42):7752-7777.
[13] T.S. Sreeprasad;Shihabudheen M. Maliyekkal;K.P. Lisha;T. Pradeep .Reduced graphene oxide-metal/metal oxide composites: Facile synthesis and application in water purification[J].Journal of hazardous materials,2011(1):921-931.
[14] 敏世雄,吕功煊.CdS/石墨烯复合材料的制备及其可见光催化分解水产氢性能[J].物理化学学报,2011(09):2178-2184.
[15] Dandapat A;De G .Host-mediated synthesis of cobalt aluminate/γ-alumina nanoflakes:A dispersible composite pigment with high catalytic activities[J].ACS Applied Materials& Interfaces,2012,4(1):228-234.
[16] K. M. Parida;Amaresh C. Pradhan .Fe/meso-Al2O3: An Efficient Photo-Fenton Catalyst for the Adsorptive Degradation of Phenol[J].Industrial & Engineering Chemistry Research,2010(18):8310-8318.
[17] Amaresh C. Pradhan;K. M. Parida .Facile synthesis of mesoporous composite Fe/Al2O3-MCM-41: an efficient adsorbent/catalyst for swift removal of methylene blue and mixed dyes[J].Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology,2012(15):7567-7579.
[18] Hummers William S;Offeman Richard E.Preparation of graphitic oxide[J].Journal of the American Chemical Society,1958(80):1339.
[19] 傅翠梨,陈文瑞,郭阿明,李锦堂,罗学涛.邻菲啰啉光度法测定高岭土中可溶铁和非可溶铁[J].岩矿测试,2012(04):621-626.
[20] HJ/T 399-2007.水质化学需氧量的测定快速消解分光光度法[S].北京:中国环境科学出版社,2008.
[21] Tingting Wu;James D. Englehardt .A New Method for Removal of Hydrogen Peroxide Interference in the Analysis of Chemical Oxygen Demand[J].Environmental Science & Technology: ES&T,2012(4):2291-2298.
[22] 宋秀丽,康杰,吕飞,穆丽荣,张卓强,秦小丹.苯酚与其降解中间产物分离的高效液相色谱法研究[J].太原师范学院学报(自然科学版),2014(02):79-83.
[23] Wei Ma;Zihong Cheng;Zhanxian Gao.Study of hydrogen gas production coupled with phenol electrochemical oxidation degradation at different stages[J].Chemical engineering journal,2014:167-174.
[24] Gentili A;Marchese S;Perret D .MS techniques for analyzing phenols, their metabolites and transformation products of environmental interest[J].TrAC: Trends in Analytical Chemistry,2008(10):888-903.
[25] LC-MS/MS analysis of phenols for classification of red wine according to geographic origin, grape variety and vintage[J].Food Chemistry,2010(1):p.366.
[26] 闫琰,叶芝祥,闫军,黄登盛.紫外光谱法同时测定水中苯酚、邻苯二酚和间苯二酚[J].化学分析计量,2008(02):22-24.
[27] Min Xia;Mingce Long;Yudong Yang.A highly active bimetallic oxides catalyst supported on Al-containing MCM-41 for Fenton oxidation of phenol solution[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2011:118-125.
[28] Pang S;Jiang J;Ma J .Oxidation of sulfoxides and arsenic(III) in corrosion of nanoscale zero valent iron by oxygen:Evidence against Ferryl ions (Fe (IV[J].Environmental Science and Technology,2011,45(1):307-312.
[29] Shuchen Hsieh;Pei-Ying Lin .FePt nanoparticles as heterogeneous Fenton-like catalysts for hydrogen peroxide decomposition and the decolorization of methylene blue[J].Journal of nanoparticle research: An interdisciplinary forum for nanoscale science and technology,2012(6):956-1-956-10.
[30] Y. Segura;F. Martinez;J.A. Melero.Enhancement of the advanced Fenton process (Fe~0/H2O2) by ultrasound for the mineralization of phenol[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2012:100-106.
[31] 褚衍洋,李玲玲,付融冰.Fenton试剂氧化苯酚过程中Fe(Ⅱ)浓度的变化[J].环境工程学报,2008(08):1057-1061.
[32] Xu Zhang;Feng Wu;Nansheng Deng .EVIDENCE OF THE HYDROXYL RADICAL FORMATION UPON THE PHOTOLYSIS OF AN IRON-RICH CLAY IN AQUEOUS SOLUTIONS[J].Reaction kinetics & catalysis letters,2008(2):207-218.
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