采用等量浸渍法以γ-Al2O3为载体,制备过渡金属Cu和Fe、贵金属Ru、稀土金属La的复合催化剂.采用催化湿式空气氧化法处理模拟印染废水,研究金属离子配比、焙烧温度对催化剂活性及稳定性的影响,并对催化剂CWAO反应机理进行探讨:权衡催化剂的活性和稳定性,催化剂的组分质量配比和焙烧温度分别为Cu∶ Fe∶ Ru∶ La=1∶1∶1∶3、450℃.对催化剂进行XRD、XPS、孔结构、FT-IR、TG-DTA、SEM、TEM表征,结果表明:焙烧使催化剂组成物质分解为氧化物,元素Cu、Fe、Ru、La分别以CuO、Fe2O3、RuO2、La2O3形式存在；焙烧温度升高,晶粒长大结晶趋于完整,催化剂孔容孔径增大但比表面积减小,晶粒尺寸分布在5～ 20 nm; Cu-Fe-Ru-La/γ-Al2O3催化剂使用前后结构无明显变化且反应后溶出的金属浓度低,催化剂具有较高的稳定性.
参考文献
| [1] | D. Rajkumar;Jong Guk Kim .Oxidation of various reactive dyes with in situ electro-generated active chlorine for textile dyeing industry wastewater treatment[J].Journal of hazardous materials,2006(2):203-212. |
| [2] | Ipek Gulkaya;Gulerman A. Surucu;Filiz B. Dilek .Importance of H_2O_2/Fe~(2+) ratio in Fenton's treatment of a carpet dyeing wastewater[J].Journal of hazardous materials,2006(3):763-769. |
| [3] | Yang Zhang;Dongliu Li;Yang Chen .Catalytic wet air oxidation of dye pollutants by polyoxomolybdate nanotubes under room condition[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2009(3/4):182-189. |
| [4] | 张永利,胡筱敏,李红.铜负载湿式氧化催化剂焙烧条件的研究[J].人工晶体学报,2010(01):272-276. |
| [5] | T. Granato;A. Katovic;K. Maduna Valkaj;A. Tagarelli;G. Giordano .Cu-silicalite-1 catalyst for the wet hydrogen peroxide oxidation of phenol[J].Journal of porous materials,2009(2):227-232. |
| [6] | R.LEVI;M.MILMAN;M.V.LANDAU .Catalytic Wet Air Oxidation of Aniline with Nanocasted Mn-Ce-Oxide Catalyst[J].Environmental Science & Technology: ES&T,2008(14):5165-6170. |
| [7] | Ovejero G;Sotelo JL;Rodriguez A;Diaz C;Sanz R;Garcia J .Platinum catalyst on multiwalled carbon nanotubes for the catalytic wet air oxidation of phenol[J].Industrial & Engineering Chemistry Research,2007(20):6449-6455. |
| [8] | 李常丽,张庆红,王野,万惠霖.限域于SBA-15孔道内的活性相聚集形态[J].催化学报,2008(01):37-40. |
| [9] | Liu Y;Sun DZ .Development of Fe2O3-CeO2-TiO2/gamma-Al2O3 as catalyst for catalytic wet air oxidation of methyl orange azo dye under room condition[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(3/4):205-211. |
| [10] | Haoxi Wu;Haijuan Li;Yujuan Zhai;Xiaolong Xu;Yongdongjin .Facile Synthesis of Free-Standing Pd-Based Nanomembranes with Enhanced Catalytic Performance for Methanol/Ethanol Oxidation[J].Advanced Materials,2012(12):1594-1597. |
| [11] | A.Quintanilla;J.A.Casas;J.J.Rodriguez .Catalytic wet air oxidation of phenol with modified activated carbons and Fe/activated carbon catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(1/2):135-145. |
| [12] | G. H. Zohuri;S. Damavandi;E. Dianat .Late Transition Metal Catalyst Based on Cobalt for Polymerization of Ethylene[J].International Journal of Polymeric Materials,2011(9/11):776-786. |
| [13] | Sen, S.S.;Hey, J.;Herbst-Irmer, R.;Roesky, H.W.;Stalke, D. .Striking stability of a substituted silicon(II) bis(trimethylsilyl)amide and the facile Si-Me bond cleavage without a transition metal catalyst[J].Journal of the American Chemical Society,2011(31):12311-12316. |
| [14] | Singaram Vengatesan;Eunae Cho;In-Hwan Oh .Development of non-precious oxygen reduction reaction catalyst for polymer electrolyte membrane fuel cells based on substituted cobalt porphyrins[J].The Korean journal of chemical engineering,2012(5):621-626. |
| [15] | Jana Mikulova;Sylvie Rossignol;Jacques Barbier Jr. .Characterizations of platinum catalysts supported on Ce, Zr,Pr-oxides and formation of carbonate species in catalytic wet air oxidation of acetic acid[J].Catalysis Today,2007(3/4):185-190. |
| [16] | Zhibin Yang,Yunyan Zhang,Weizhong Ding,Yuwen Zhang,Peijun Shen,Yuding Zhou,Yong Liu,Shaoqing Huang,Xionggang Lu.Hydrogen production from coke oven gas over LiNi/γ-Al_2O_3 catalyst modified by rare earth metal oxide in a membrane reactor[J].天然气化学（英文版）,2009(04):407-414. |
| [17] | 朱林,曹立新,苏革,柳伟,刘辉,宋亮.稀土Gd3+掺杂TiO2纳米带的制备及其光催化性能研究[J].人工晶体学报,2011(03):579-583. |
| [18] | 郑好转,王梅柳,华卫琦,翁维正,伊晓东,黄传敬,万惠霖.焙烧气氛对Ru/Al2O3催化剂上甲烷部分氧化制合成气反应性能的影响[J].催化学报,2011(01):93-99. |
| [19] | M. Mazurek;N. Benker;C. Roth;H. Fuess .Binary Mixtures of Carbon Supported Pt and Ru Catalysts for PEM Fuel Cells[J].Fuel cells,2006(3/4):208-213. |
| [20] | K. LIDDELL;D.P.THOMPSON;T. BRAUNIGER .M_2(Si,Al)_4(N,C)_7 (M = La,Y,Ca) carbonitrides. I. Synthesis and structural characterisation by XRD and NMR[J].Journal of the European Ceramic Society,2005(1):37-47. |
| [21] | Yurieva TM;Plyasova LM;Zaikovskii VI;Minyukova TP;Bliek A;van den Heuvel JC;Davydova LP;Molina IY;Demeshkina MP;Khassin AA .In situ XRD and HRTEM studies on the evolution of the Cu/ZnO methanol synthesis catalyst during its reduction and re-oxidation[J].Physical chemistry chemical physics: PCCP,2004(18):4522-4526. |
| [22] | S.C. Chanda;A. Manna;V. Vijayan .PIXE & XRD analysis of nanocrystals of Fe, Ni and Fe_2O_3[J].Materials Letters,2007(28):5059-5062. |
| [23] | Haverkamp, R.G.;Marshall, A.T.;Cowie, B.C.C. .Energy resolved XPS depth profile of (IrO_2, RuO_2, Sb_2O_5, SnO_2) electrocatalyst powder to reveal core-shell nanoparticle structure[J].Surface and Interface Analysis: SIA: An International Journal Devoted to the Development and Application of Techniques for the Analysis of Surfaces, Interfaces and Thin Films,2011(5):847-855. |
| [24] | 陈启元,童海霞,尹周澜,胡慧萍,李洁,刘亮亮.氧缺位型TiO2的制备、表征及其光催化析氧活性[J].物理化学学报,2007(12):1917-1921. |
| [25] | Lei Huang;Feng Peng;Fumio S. Ohuchi .'In situ' XPS study of band structures at Cu_2O/TiO_2 heterojunctions interface[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,2009(17):2815-2819. |
| [26] | Sakai, Y.;Ninomiya, S.;Hiraoka, K. .XPS depth analysis of CuO by electrospray droplet impact[J].Surface and Interface Analysis: SIA: An International Journal Devoted to the Development and Application of Techniques for the Analysis of Surfaces, Interfaces and Thin Films,2012(8):938-941. |
| [27] | Kalinkin A.V.;Savchenko,V.I. .Mechanism of low-temperature CO oxidation on a model Pd/Fe_2O_3 catalyst[J].Catalysis Letters,1999(2/4):115-119. |
| [28] | J. P. Espinos;J. Morales;A. Barranco;A. Caballero;J. P. Holgado;A. R. Gonzalez-Elipe .Interface Effects for Cu, CuO, and Cu_2O Deposited on SiO_2 and ZrO_2. XPS Determination of the Valence State of Copper in Cu/SiO_2 and Cu/ZrO_2 Catalysts[J].The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical,2002(27):6921-6929. |
| [29] | D.L.Hoang;A.Dittmar;J.Radnik;K.-W.Brzezinka;K.Witke .Redox behaviour of La-Cr compounds formed in CrO_x/La_2O_3 mixed oxides and CrO_x/La_2O_3/ZrO_2 catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2003(1/2):95-110. |
| [30] | Co/mg/al Hydrotalcite-type Precursor, Promoted With La And Ce, Studied By Xps And Applied To Methane Steam Reforming Reactions[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,2009(11):5851-5856. |
| [31] | Khodakov, AY;Zholobenko, VL;Bechara, R;Durand, D .Impact of aqueous impregnation on the long-range ordering and mesoporous structure of cobalt containing MCM-41 and SBA-15 materials[J].Microporous and Mesoporous Materials,2005(1/3):29-39. |
| [32] | Khodakov AY.;Griboval-Constant A.;Bechara R.;Zholobenko VL. .Pore size effects in Fischer Tropsch synthesis over cobalt-supported mesoporous silicas[J].Journal of Catalysis,2002(2):230-241. |
| [33] | 李常丽,张庆红,王野,万惠霖.限域于SBA-15孔道内的活性相聚集形态[J].催化学报,2008(01):37-40. |
| [34] | Bengisu M;Brow RK;Yimaz E;Mogus-Milankovic A;Reis ST .Aluminoborate and aluminoboro silicate glasses with high chemical durability and the effect Of P2O5 additions on the properties[J].Journal of Non-Crystalline Solids: A Journal Devoted to Oxide, Halide, Chalcogenide and Metallic Glasses, Amorphous Semiconductors, Non-Crystalline Films, Glass-Ceramics and Glassy Composites,2006(32/35):3668-3676. |
| [35] | A. A. Egorov;M. A. Semin .HIGH-POROSITY CELLULAR MATERIALS BASED ON ALKALI ALUMINOBOROSILICATE GLASS[J].Glass and ceramics,2007(5/6):190-192. |
| [36] | 张桂银,毕淑琴,董元彦,李丽仙,李学垣.有机酸对针铁矿和三羟铝石吸附镉离子的影响[J].河北农业大学学报,2002(04):49-52. |
| [37] | Grossl PR;Sparks DL .EVALUATION FOR CONTAMINANT ION ADSORPTION DESORPTION ON GOETHITE USING PRESSURE-JUMP RELAXATION KINETICS[J].Geoderma: An International Journal of Soil Science,1995(1/2):87-101. |
| [38] | M.Bengisu;E.Yilmaz;H.Farzad .Borate,lithium borate,and borophosphate powders by sol-gel precipitation[J].Journal of Sol-Gel Science and Technology,2008(3):237-243. |
| [39] | Ohman M;Persson D;Leygraf C .In situ ATR-FTIR studies of the aluminium/polymer interface upon exposure to water and electrolyte[J].Progress in Organic Coatings: An International Review Journal,2006(1):78-88. |
| [40] | Vedprakash S. Mishra;Vijaykumar V. Mahajani;Jyeshtharaj B. Joshi .Wet Air Oxidation[J].Industrial & Engineering Chemistry Research,1995(1):2-48. |
| [41] | 杨少霞,冯玉杰,万家峰,蔡伟民,祝万鹏,蒋展鹏.CeO2掺杂RuO2/γ-Al2O3催化剂结构与湿式氧化降解苯酚的活性研究[J].高等学校化学学报,2005(05):897-901. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%