In order to investigate the influence of MnO2 modification methods on the catalytic performance of CuO/CeO2 catalyst for NO reduction by CO, two series of catalysts (xCuyMn/Ce and xCu/yMn/Ce) were prepared by co-impregnation and step-wise-impregnation methods, and characterized by means of X-ray diffraction (XRD), Raman spectra, H2-temperature programmed reduction (H2-TPR), in situ diffuse reflectance infrared Fourier transform spectra (in situ DRIFTS) techniques. Furthermore, the cata-lytic performances of these catalysts were evaluated by NO+CO model reaction. The obtained results indicated that:(1) The catalysts acquired by co-impregnation method exhibited stronger interaction owing to the more sufficient contact among each component of the catalysts compared with the catalysts obtained by stepwise-impregnation method, which was beneficial to the improvement of the reduction behavior;(2) The excellent reduction behavior was conducive to the formation of low valence state copper species (Cu+/Cu0) and more oxygen vacancies (especially the surface synergetic oxygen vacancies (SSOV, Cu+-Mn(4-x)+)) during the reaction process, which were beneficial to the adsorption of CO species and the dissociation of NO species, respectively, and further promoted the en-hancement of the catalytic performance. Finally, in order to further understand the difference between the catalytic performances of these catalysts prepared by co-impregnation and stepwise-impregnation methods, a possible reaction mechanism (schematic diagram) was tentatively proposed.
参考文献
[1] | Chen J F;Zhu J J;Zhan Y Y;Lin X Y,Cai G H,Wei K M,Zhen Q .Characterization and catalytic performance of Cu/CeO2 and Cu/MgO-CeO2 catalysts for NO reduction by CO[J].Appl Catal A,2009,363(1-2):208. |
[2] | Granger P;Lecomte J J;Leclercq L;Leclercq G .An at-tempt at modelling the activity of Pt-Rh/Al2O3 three-way catalysts in the CO+NO reaction[J].Appl Catal A,2001,208(1-2):369. |
[3] | Cónsul J M D;Costilla I;Gigola C E;Baibich I M .NO reduction with CO on alumina-modified silica-supported palladium and molybdenum-palladium catalysts[J].Appl Catal A,2008,339(02):151. |
[4] | Araya P;Gracia F;Cortés J;Wolf E E .FTIR study of the reduction reaction of NO by CO over Rh/SiO2 catalysts with different crystallite size[J].Appl Catal B,2002,38(02):77. |
[5] | Nováková J;Kubelková L .Contribution to the mechanism of NO reduction by CO over Pt/NaX zeolite[J].Appl Catal B,1997,14(3-4):273. |
[6] | Zhu H O;Kim J R;Ihm S K .Characteristics of Pt/WO3/CeO2/ZrO2 catalysts for catalytic reduction of NO by CO[J].Appl Catal B,2009,86(1-2):87. |
[7] | Jean-Luc Freysz;Jacques Saussey;Jean-Claude Lavalley .In Situ FTIR Study of the NO +CO Reaction on a Silica-Supported Platinum Catalyst at Atmospheric Pressure Using a New Pulse Technique[J].Journal of Catalysis,2001(1):131-138. |
[8] | Yao X J;Yu Q;Ji Z Y;Lv Y Y,Cao Y,Tang C J,Gao F,Dong L,Chen Y .A comparative study of different doped metal cations on the reduction,adsorption and activity of CuO/Ce0.67M0 33O2(M=Zr4+,Sn4+,Ti4+)catalysts for NO+CO reaction[J].Appl Catal B,2013,130-131(0):293. |
[9] | Jiang X Y;Lou L P;Ding G H;Chen Y X Zheng X M .The active species and catalytic properties of CuO/CeO2-TiO2 catalysts for NO+CO reaction[J].Journal of Materials Science,2004,39(14):4663. |
[10] | Reddy B M;Lakshmanan P;Khan A .Investigation of sur-face structures of dispersed V2O5 on CeO2-SiO2,CeO2-TiO2,and CeO2-ZrO2 mixed oxides by XRD,Raman,and XPS techniques[J].Journal of Physical Chemistry B,2004,108(43):16855. |
[11] | Xiaojiang Yao;Changjin Tang;Zeyang Ji .Investigation of the physicochemical properties and catalytic activities of Ce_(0.67)M_(0.33)O2 (M = Zr~(4+), Ti~(4+), Sn~(4+)) solid solutions for NO removal by CO[J].Catalysis science & technology,2013(3):688-698. |
[12] | Yu, Q.;Wu, X.;Tang, C.;Qi, L.;Liu, B.;Gao, F.;Sun, K.;Dong, L.;Chen, Y. .Textural, structural, and morphological characterizations and catalytic activity of nanosized CeO_2-MO_x (M=Mg~(2+), Al~(3+), Si~(4+)) mixed oxides for CO oxidation[J].Journal of Colloid and Interface Science,2011(1):341-352. |
[13] | Jiang X Y;Jia Y R;Huang H;Zheng X M .Effect of pre-treatment atmosphere on CuO/TiO2 activities in NO+CO reaction[J].Catalysis Letters,2005,104(03):169. |
[14] | Liu L J;Cai J G;Qi L;Yu Q,Sun K Q,Liu B,Gao F,Dong L,Chen Y .Influence of supports structure on the ac-tivity and adsorption behavior of copper-based catalysts for NO reduction[J].J Mol Catal A,2010,327(1-2):1. |
[15] | Hu Y H;Dong L;Shen M M;Liu D,Wang J,Ding W P,Chen Y .Influence of supports on the activities of copper oxide species in the low-temperature NO+CO reaction[J].Appl Catal B,2001,31(01):61. |
[16] | Invanka Spassova;Mariana Khristova;Dimitar Panalyotov;Dimitar Mehandjiev .Coprecipitated CuO-MnO_x Catalysts for Low-Temperature CO-NO and CO-NO-O_2 Reactions[J].Journal of Catalysis,1999(1):43-57. |
[17] | Ivanka Spassova;Dimitar Mehandjiev .Mechanism of no conversion over a coprecipitated CuO_MnOx spinel-like catalyst[J].Reaction kinetics & catalysis letters,2000(2):231-237. |
[18] | Spassova I;Khristova M;Nickolov R;Mehandjiev D .Novel application of depleted fullerene soot (DFS) as support of catalysts for low-temperature reduction of NO with CO[J].Journal of Colloid and Interface Science,2008(1):186-193. |
[19] | Liu, L.;Yu, Q.;Zhu, J.;Wan, H.;Sun, K.;Liu, B.;Zhu, H.;Gao, F.;Dong, L.;Chen, Y. .Effect of MnO_x modification on the activity and adsorption of CuO/Ce_(0.67)Zr_(0.33)O_2 catalyst for NO reduction[J].Journal of Colloid and Interface Science,2010(1):246-255. |
[20] | A. Gurbani;J. L. Ayastuy;M. P. Gonzdlez-Marcos;J. E. Herrero;J.M. Guil;M. A. Gutierrez-Ortiz .Comparative Study Of Cuo-ceo_2 Catalysts Prepared By Wet Impregnation And Deposition-precipitation[J].International journal of hydrogen energy,2009(1):547-553. |
[21] | Duan K J;Tang X L;Yi H H;Ning P Wang L D .Rare earth oxide modified Cu-Mn compounds supported on TiO2 catalysts for low temperature selective catalytic oxi-dation of ammonia and in lean oxygen[J].Journal of Rare Earths,2010,28(Suppl 1):338. |
[22] | Yu Q;Yao X J;Zhang H L;Gao F,Dong L .Effect of ZrO2 addition method on the activity of Al2O3-supported CuO for NO reduction with CO:Impregnation vs.copre-cipitation[J].Appl Catal A,2012,423-424(0):42. |
[23] | Xiaojiang Yao;Fei Gao;Qiang Yu .NO reduction by CO over CuO-CeO2 catalysts: effect of preparation methods[J].Catalysis science & technology,2013(5):1355-1366. |
[24] | Jixin Zhu;Wenhui Shi;Ni Xiao .Oxidation-Etching Preparation of MnO2 Tubular Nanostructures for High-Performance Supercapacitors[J].ACS applied materials & interfaces,2012(5):2769-2774. |
[25] | QIAO Dongsheng,LU Guanzhong,GUO Yun,WANG Yanqin,GUO Yanglong.Effect of water vapor on the CO and CH4 catalytic oxidation over CeO2-Mox (M=Cu, Mn, Fe, Co, and Ni) mixed oxide[J].稀土学报(英文版),2010(05):742-746. |
[26] | Li T Y;Chiang S J;Liaw B J;Chen Y Z .Catalytic oxida-tion of benzene over CuO/Ce1-xMnxO2 catalysts[J].Appl Catal B,2011,103(1-2):143. |
[27] | Hong, W.-J.;Iwamoto, S.;Hosokawa, S.;Wada, K.;Kanai, H.;Inoue, M. .Effect of Mn content on physical properties of CeO_x-MnO_ y support and BaO-CeO_x-MnO_y catalysts for direct NO decomposition[J].Journal of Catalysis,2011(2):208-216. |
[28] | P. Zimmer;A. Tschope;R. Birringer .Temperature-Programmed Reaction Spectroscopy of Ceria- and Cu/Ceria-Supported Oxide Catalyst[J].Journal of Catalysis,2002(2):339-345. |
[29] | Dow WP.;Huang TJ.;Wang YP. .YTTRIA-STABILIZED ZIRCONIA SUPPORTED COPPER OXIDE CATALYST .1. EFFECT OF OXYGEN VACANCY OF SUPPORT ON COPPER OXIDE REDUCTION[J].Journal of Catalysis,1996(2):155-170. |
[30] | Dow WP.;Huang TJ. .YTTRIA-STABILIZED ZIRCONIA SUPPORTED COPPER OXIDE CATALYST .2. EFFECT OF OXYGEN VACANCY OF SUPPORT ON CATALYTIC ACTIVITY FOR CO OXIDATION[J].Journal of Catalysis,1996(2):171-182. |
[31] | Kapteijn F;Vanlangeveld A D;Moulijn J A;Andreini A Vuurman M A Turek A M Jehng J M Wachs I E .Alu-mina-supported manganese oxide catalysts:I characteri-zation:effect of precursor and loading[J].J Catal,1994,150(01):94. |
[32] | Sun C Z;Zhu J;Lü Y Y;Qi L,Liu B,Gao F,Sun K Q,Dong L,Chen Y .Dispersion,reduction and catalytic per-formance of CuO supported on ZrO2-doped TiO2 for NO removal by CO[J].Appl Catal B,2011,103(1-2):206. |
[33] | Liu L J;Liu B;Dong L H;Zhu J,Wan H Q,Sun K Q,Zhao B,Zhu H Y,Dong L,Chen Y .In situ FT-infrared investigation of CO or/and NO interaction with CuO/Ce0.67Zr0 33O2 catalysts[J].Appl Catal B,2009,90(3-4):578. |
[34] | Hadjiivanov KI. .Identification of neutral and charged NxOy surface species by IR spectroscopy [Review][J].Catalysis Reviews. Science and Engineering,2000(1/2):71-144. |
[35] | Qi L;Yu Q;Dai Y;Tang C J,Liu L J,Zhang H L,Gao F,Dong L,Chen Y .Influence of cerium precursors on the structure and reducibility of mesoporous CuO-CeO2 cata-lysts for CO oxidation[J].Appl Catal B,2012,119-120(0):308. |
[36] | Hadjiivanov K I;Vayssilov G N .Characterization of oxide surfaces and zeolites by carbon monoxide as an IR probe molecule[J].ADVANCES IN CATALYSIS,2002,47:307. |
[37] | Oh S H;Fisher G B;Carpenter J E;Goodman D W .Com-parative kinetic studies of CO-O2 and CO-NO reactions over single crystal and supported rhodium catalysts[J].J Catal,1986,100(02):360. |
[38] | Li, D.;Yu, Q.;Li, S.-S.;Wan, H.-Q.;Liu, L.-J.;Qi, L.;Liu, B.;Gao, F.;Dong, L.;Chen, Y. .The remarkable enhancement of CO-pretreated CuO??Mn _2O_3/γ-Al_2O_3 supported catalyst for the reduction of NO with CO: The formation of surface synergetic oxygen vacancy[J].Chemistry: A European journal,2011(20):5668-5679. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%