负载型催化剂具有重要的应用背景,研究表面分散组分与载体之间的相互作用.对于了解催化过程的本质,进而设计开发高效实用的催化剂均有重要的指导意义.本课题组近年来在该领域中进行了一些探索研究,涉及的催化剂以负载型金属氧化物(如CuO/γ-Al_2O_3,CuO/Ce_xZr_(1-x)O_2和CuO/Ti_xSn_(1-x)O_2等)为主,涉及的反应包括CO完全氧化和NO+CO反应.通过改变活性组分的负载量、添加改性剂和改变样品制备条件等制得一系列样品,用多种固体催化剂表征手段考察各组分在催化剂中的作用以及在上述催化反应中的活性变化规律.研究表明:(1)金属氧化物和卤化物等离子化合物在氧化物载体表面的分散容量和分散后的一些性质均可从"嵌入模型"的考虑得到解释;(2)处于不同载体表面的活性物种或同一载体表面不同结构的活性物种,由于其存在状态的差异使得其氧化还原性质和催化性质不同;(3)在相关催化剂体系中进行的CO完全氧化和NO+CO反应的结果显示,通过探索催化剂的"组成-结构-性质"间的关系,有可能为实际催化剂的设计提供理论参考.
Supported catalysts are widely used in industry and in academic research, and the investigation of the interaction between the dispersed surface components and supports is key to the understanding of the nature of catalytic reactions and the design and development of effective and practical catalysts. This review summarizes some results of our group in this field. The related catalysts include supported metal oxides such as CuO/γ-Al_2O_3, CuO/Ce_xZr_(1-x)O_2, and CuO/Ti_xSn_(1-x)O_2, and the reactions are mainly focused on the CO oxidation and NO + CO reaction. These mentioned catalysts, prepared by adjusting the Ioadings of active species, introducing modifiers, and changing preparation conditions, are characterized by normal measurements for solid catalysts in order to explore the functions of each component and monitor the variation of activity in the reactions. It is shown that: (1) the dispersion capacity of metal oxides or halides on the surface of oxide supports and some of their properties can be explained on the basis of the "incorporation model"; (2) the dispersed active species on the different supports or the dispersed active species with different structures on the same support exhibit different redox and catalytic properties, which are resulted from the diversity of tbeir existing states; (3) the results obtained from CO oxidation and NO + CO reactions proceeding on the associated catalysts indicate that it is possible to design catalysts by exploring the relationship among "composition-structure-property".
参考文献
| [1] | Sheintuch M;Schmidt J;Lechtman Y;Yahav G .[J].Applied Catalysis,1989,49:55. |
| [2] | Thormahlen P;Skoglundh M;Fridell E;Andwesson B .[J].Journal of Catalysis,1999,188:300. |
| [3] | Fernandez-Garcia M;Martinez-Arias A;Salamanca L N;Coronado J M Anderson J A Conesa J C Soria J .[J].Journal of Catalysis,1999,187:474. |
| [4] | Sayo K;Deki S;Hayashi S .[J].Journal of Materials Chemistry,1999,9:937. |
| [5] | Manuel I;Thomas C;Bourgeois C;Colas H Matthess N Djega-Mariadassou G .[J].Catalysis Letters,2001,77:193. |
| [6] | Gervasini A;Carniti P;Ragaini V .[J].Applied Catalysis B:Environmental,1999,22:201. |
| [7] | Nakamura I.;Fujitani T.;Hamada H. .Adsorption and decomposition of NO on Pd surfaces[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,2002(1/3):409-413. |
| [8] | Pietraszek A;Costa P D;Marques R;Kornelak P Hansen T W Camra J Najbar M .[J].Catalysis Today,2007,119:187. |
| [9] | Kummer J T .[J].Progress in Energy and Combustion Science,1980,6:177. |
| [10] | Severino F;Brito J;Carias O;Laine J .[J].Journal of Catalysis,1986,102:172. |
| [11] | Park P W;Ledford J S .[J].Applied Catalysis B:Environmental,1998,15:221. |
| [12] | Cao J L;Wang Y;Zhang T Y;Wu S H Yuan Z Y .[J].Applied Catalysis B:Environmental,2008,78:120. |
| [13] | Jansson J;Skoglundh M;Fridell E;Thormahlen P .[J].Topics in Catalysis,2001,16:385. |
| [14] | Radwan N R E .[J].Applied Catalysis A:General,2004,257:177. |
| [15] | Craciun R. .Structure/activity correlation for unpromoted and CeO2-promoted MnO2/SiO2 catalysts[J].Catalysis Letters,1998(1):25-31. |
| [16] | Zhang R D;Alamdari H;Kaliaguine S .[J].Journal of Catalysis,2006,242:241. |
| [17] | Jiang X Y;Ding G H;Lou L P;Chen Y X Zheng X M .[J].J Mol CatalA,2004,218:187. |
| [18] | Bhargava SK;Akolekar DB .Adsorption of NO and CO over transition-metal-incorporated mesoporous catalytic materials[J].Journal of Colloid and Interface Science,2005(1):171-178. |
| [19] | Wen B;He M Y .[J].Applied Catalysis B:Environmental,2002,37:75. |
| [20] | Amano F;Suzuki S;Yamamoto T;Tanaka T .One-electron reducibility of isolated copper oxide on alumina for selective NO-CO reaction[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(3/4):282-289. |
| [21] | Pantazis CC;Petrakis DE;Pomonis PJ .Simultaneous and/or separate SO2/NO reduction by CO over high surface area Cu/Ce containing mesoporous silica[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(1/2):66-72. |
| [22] | Selwood P W .[J].Advances in Catalysis,1951,3:27. |
| [23] | Iwasawa Y .[J].Studies in Surface Science and Catalysis,1996,101:21. |
| [24] | Olth of B;Khodakov A;Bell A T;Iglesia E .[J].Journal of Physical Chemistry B,2000,104:1516. |
| [25] | Xie S B;Iglesia E;Bell A T .[J].Journal of Physical Chemistry B,2001,105:5144. |
| [26] | Xie SB.;Bell AT.;Iglesia E. .Effects of hydration and dehydration on the structure of silica-supported vanadia species[J].Langmuir: The ACS Journal of Surfaces and Colloids,2000(18):7162-7167. |
| [27] | Cheung P;Liu H C;Iglesia E .[J].Journal of Physical Chemistry B,2004,108:18650. |
| [28] | Dai H X;Bell A T;Iglesia E .[J].Journal of Catalysis,2004,221:491. |
| [29] | Knozinger H;Taglauer E;Spivey J J;Agarwal S K.Catalysis[M].Cambridge:The Royal Society of Chemistry,1993:1. |
| [30] | Wu M;Hercules D M .[J].Journal of Physical Chemistry,1979,83:2003. |
| [31] | Strohmeier B R;Levden D E;Field R S;Hercules D M .[J].Journal of Catalysis,1985,94:514. |
| [32] | Wachs I E .[J].Catalysis Today,1996,27:437. |
| [33] | Hardcastle F D;Wachs 1 E;Horsley J A;Via G H .[J].Journal of Molecular Catalysis,1988,46:15. |
| [34] | Wang X;Wachs I E .[J].Catalysis Today,2004,96:211. |
| [35] | Tian H J;Wachs I E;Briand L E .[J].Journal of Physical Chemistry B,2005,109:23491. |
| [36] | Coluccia S;Marchese L .[J].Catalysis Today,1998,41:229. |
| [37] | Reddy B M;Sreekanth P M;Yamada Y;Xu Q Kobayashi T .[J].Applied Catalysis A:General,2002,228:269. |
| [38] | Reddy B M;Chowdhury B;Smirniotis P G .[J].Applied Catalysis A:General,2001,211:19. |
| [39] | Reddy BM.;Chowdhury B. .Dispersion and thermal stability of MoO3 on TiO2-ZrO2 mixed oxide support[J].Journal of Catalysis,1998(2):413-419. |
| [40] | Xie Y C;Tang Y Q .[J].Advances in Catalysis,1990,37:1. |
| [41] | Yan J H;Liu Y J;Gui L L;Tang Y Q .[J].Ada Phys-Chim Sin,1993,9:13. |
| [42] | 罗胜成;桂琳琳;罗锡辉.[J].物理化学学报,1996(02):341. |
| [43] | 傅贤智;罗胜成;桂琳琳;罗锡辉 .[J].化学学报,1992,50:342. |
| [44] | 傅贤智;罗胜成;桂琳琳;唐有祺.[J].自然科学进展,1991(01):543. |
| [45] | Goodman DW. .Model catalysts: from imagining to imaging a working surface[J].Journal of Catalysis,2003(1/2):213-222. |
| [46] | Hess C;Ozensoy E;Goodman D W .[J].Journal of Physical Chemistry B,2003,107:2759. |
| [47] | Xu C;Oh W S;Goodman D W .[J].Journal of Physical Chemistry B,2000,104:10310. |
| [48] | Chen M S;Santra A K;Goodman D W .[J].Journal of Physical Chemistry B,2004,108:17940. |
| [49] | Chen MS;Goodman DW .The structure of catalytically active gold on titania[J].Science,2004(5694):252-255. |
| [50] | Chen Y;Zhang L F;Lin J F;Jin Y S .[J].Catalysis Science and Technology,1990,1:291. |
| [51] | Chen Y;Zhang L F .[J].Catalysis Letters,1992,12:51. |
| [52] | Gates B C;Katzer J R;Schuit G C A.Chemistry of Catalytic Processes[M].New York:McGraw-Hill,1979 |
| [53] | Beaufils J P;Barbaux Y .[J].Journal of Chemical Physics,1981,78:347. |
| [54] | Jimenez-Gonzalez A;Schmeisser D .[J].Surface Science,1991,250:59. |
| [55] | Chen Y;Zhang L F;Lin J F;Jin Y S .[J].Catalysis Science and Technology,1991,1:291. |
| [56] | Wan H Q;Wang Z;Zhu J;Li X W Liu B Gao F Dong L Chen Y .[J].Applied Catalysis B:Environmental,2008,79:254. |
| [57] | Larsson P O;Andersson A .[J].Applied Catalysis B:Environmental,2000,24:175. |
| [58] | Hu Y H;Dong L;Wang J;Ding W P Chen Y .[J].Journal of Molecular Catalysis A:Chemical,2000,162:307. |
| [59] | 万海勤 .[D].南京:南京大学,2008. |
| [60] | Liu W;Sar of im A F;Flytzani-Stephanopoulos M .[J].Chemical Engineering Science,1995,49:4871. |
| [61] | Liu W.;Flytzanistephanopoulos M. .TOTAL OXIDATION OF CARBON MONOXIDE AND METHANE OVER TRANSITION METAL-FLUORITE OXIDE COMPOSITE CATALYSTS .1. CATALYST COMPOSITION AND ACTIVITY[J].Journal of Catalysis,1995(2):304-316. |
| [62] | Yamashita T.;Vannice A. .N2O DECOMPOSITION OVER MANGANESE OXIDES[J].Journal of Catalysis,1996(1):254-262. |
| [63] | Yamashita T.;Vannice A. .NO DECOMPOSITION OVER MN2O3 AND MN3O4[J].Journal of Catalysis,1996(1):158-168. |
| [64] | Spassova I;Khristova M;Panayotov D;Mehandjiev D .[J].Journal of Catalysis,1999,185:43. |
| [65] | Tikhomirov K;Krcher O;Elsener M;Wokaun A .[J].Applied Catalysis B:Environmental,2006,64:72. |
| [66] | Lamb A B;Bray W C;Frazer J C W .[J].Journal of Industrial and Engineering Chemistry,1920,12:213. |
| [67] | Chen HY.;Tan KL.;Li J.;Lin J. .Comparative studies of manganese-doped copper-based catalysts: the promoter effect of Mn on methanol synthesis[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,1998(3/4):323-331. |
| [68] | Phil HH;Reddy MP;Kumar PA;Ju LK;Hyo JS .SO2 resistant antimony promoted V2O5/TiO2 catalyst for NH3-SCR of NOx at low temperatures[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(3/4):301-308. |
| [69] | Vargas MAL;Casanova M;Trovarelli A;Busca G .An IR study of thermally stable V2O5-WO3-TiO2SCR catalysts modified with silica and rare-earths (Ce, Tb, Er)[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(3/4):303-311. |
| [70] | Stranick M A;Houalla M;Hercules D M .[J].Journal of Catalysis,1987,106:362. |
| [71] | Wang J;Dong L;Hu Y H;Zheng G S Hu Z Chen Y .[J].Journal of Solid State Chemistry,2001,157:274. |
| [72] | Hu Y H;Liu T D;Shen M M;Zhu H Y Wei S T Hong X Ding W P Dong L Chen Y .[J].Journal of Solid State Chemistry,2003,170:58. |
| [73] | 杨立娟,李晓伟,刘斌,万海勤,胡玉海,董林.MO（M=Cu和Ni）/TiO2/-Al2O3催化剂在CO+O2反应中的活性[J].无机化学学报,2007(10):1717-1722. |
| [74] | Chernavskii P.A.;Pankina G.V. .The influence of oxide-oxide interaction on the catalytic properties of Co/Al_2O_3 in CO hydrogenation[J].Catalysis Letters,2000(3):121-124. |
| [75] | Wang Z;Wan HQ;Liu B;Zhao X;Li XW;Zhu HY;Xu X;Ji FY;Sun KQ;Dong L .Influence of magnesia modification on the properties of copper oxide supported on gamma-alumina[J].Journal of Colloid and Interface Science,2008(2):520-526. |
| [76] | Zhu H Y;Shen M M;Gao F;Kong Y Dong L Chen Y Jian C Liu Z .[J].Catalysis Communications,2004,5:453. |
| [77] | Arnoldy P;Moulijn J A .[J].Journal of Catalysis,1985,93:38. |
| [78] | Wan H Q;Li D;Dai Y;Hu Y H Zhang Y H Liu L J Zhao B Liu B Sun K Q Dong L Chen Y .[J].Applied Catalysis A:General,2009,360:26. |
| [79] | 徐斌;董林;陈懿;张鸿斌,蔡俊修,廖代伟,万惠霖.催化研究进展[M].厦门:厦门大学出版社,1996:582. |
| [80] | Zhang L F;Lin J F;Chen Y .[J].Journal of Solid State Chemistry,1992,97:292. |
| [81] | 董林;陈懿 .[J].催化学报,1995,16:85. |
| [82] | 董林 .[D].南京:南京大学,1995. |
| [83] | Chen Y;Dong L;Jin Y S;Xu B Ji W J .[J].Studies in Surface Science and Catalysis,1996,101:1293. |
| [84] | Trovarelli A .[J].Catalysis Review:Science and Engineering,1996,38:439. |
| [85] | Khaodee W;Jongsomjit B;Assabummngrat S;Praserthdam P Goto S .[J].Catalysis Communications,2007,8:548. |
| [86] | Hilaire S;Wang X;Luo T;Gorte R J Wagner J .[J].Applied Catalysis A:General,2001,215:271. |
| [87] | Wang X;Gorte R J .[J].Applied Catalysis A:General,2002,224:209. |
| [88] | Cochrane H D;Hutchison J L;White D .[J].Ultramicroscopy,1989,31:138. |
| [89] | Liu Z.;Chen Y. .Spectroscopic studies on tetragonal ZrO2-supported MoO3 and NiO-MoO3 systems[J].Journal of Catalysis,1998(2):314-324. |
| [90] | Dong L;Hu Y H;Shen M M;Jin T Wang J Ding W P Chen Y .[J].CHEMISTRY OF MATERIALS,2001,13:4227. |
| [91] | 董林;金永漱;陈懿 .[J].中国科学A辑,1997,40:24. |
| [92] | 董林;胡静秋;徐斌;陈懿 .[J].科学通报,1997,42:1405. |
| [93] | Dong L;Hu J Q;Xu B;Chen Y .[J].Chinese Science Bulletin,1997,42:1278. |
| [94] | Dong L;Chen Y .[J].Journal of the Chemical Society,Faraday Transactions,1996,92:4589. |
| [95] | Du X Z;Dong L;Li C;Liang Y Q Chen Y .[J].Langmuir,1999,15:1693. |
| [96] | Dong L;Hu Y H;Xu F;Lu D Xu B Hu Z Chen Y .[J].Journal of Physical Chemistry B,2000,104:78. |
| [97] | Chen H L;Zhu H Y;Wu Y;Gao F Dong L Zhu J J .[J].Journal of Molecular Catalysis A:Chemical,2006,255:254. |
| [98] | Hu Y H;Dong L;Shen M M;Liu D Wang J Ding W P Chen Y .[J].Applied Catalysis B:Environmental,2001,31:61. |
| [99] | Chen, HL;Zhu, HY;Wang, H;Dong, L;Zhu, JJ .Sonochemical fabrication and characterization of ceria (CeO2) nanowires[J].Journal of nanoscience and nanotechnology,2006(1):157-161. |
| [100] | 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 .[J].Applied Catalysis B:Environmental,2009,90:578. |
| [101] | Chan S S;Wachs I E;Murrell L L .[J].Journal of Catalysis,1984,90:150. |
| [102] | Di Gregorio F;Keller V .[J].Journal of Catalysis,2004,225:45. |
| [103] | Xu B;Dong L;Fan Y N;Chen Y .[J].Journal of Catalysis,2000,193:88. |
| [104] | Li X W;Shen M M;Hong X;Zhu H Y Gao F Kong Y Dong L Chen Y .[J].Journal of Physical Chemistry B,2005,109:3949. |
| [105] | Li X W;Wan H Q;Liu B;Yang L J Zhu H Y Chen H L Zhao X Sun K Q Dong L Chen Y .[J].CATALYSIS COMMUNICATIONS,2009,10:741. |
| [106] | Haneda M;Kintaichi Y;Bion N;Hamada H .[J].Applied Catalysis B:Environmental,2003,46:473. |
| [107] | Xue L;Zhang CB;He H;Teraoka Y .Catalytic decomposition of N2O over CeO2 promoted CO3O4 spinel catalyst[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(3/4):167-174. |
| [108] | Zhang Z L;Geng H R;Zheng L;Du B .[J].Journal of Alloys and Compounds,2005,392:317. |
| [109] | Iwamoto S;Takahashi R;Inoue M .Direct decomposition of nitric oxide over Ba catalysts supported on CeO2-based mixed oxides[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(26):146-150. |
| [110] | Haneda M;Kintaichi Y;Hamada H .Reaction mechanism of NO decomposition over alkali metal-doped cobalt oxide catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2005(3):169-175. |
| [111] | Asano K;Ohnishi C;Iwamoto S;Shioya Y;Inoue M .Potassium-doped CO3O4 catalyst for direct decomposition of N2O[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(3/4):242-249. |
| [112] | Sazonov B A;Popovskii V V;Boreskov G K .[J].Kinetics and Catalysis,1968,9:255. |
| [113] | Liu L J;Chen Y;Dong L H;Zhu J Wan H Q Liu B Zhao B Zhu H Y Sun K Q Dong L Chen Y .[J].Applied Catalysis B:Environmental,2009,90:105. |
| [114] | 许波连,范以宁,刘浏,林明,陈懿.Dispersion state and catalytic properties of vanadia species on the surface of V2O5/TiO2 catalysts[J].中国科学B辑(英文版),2002(04):407-415. |
| [115] | Matsuda S;Kato A .[J].Applied Catalysis,1983,8:149. |
| [116] | Reiche M A;Ortelli E;Baiker A .[J].Applied Catalysis B:Environmental,1999,23:187. |
| [117] | Dunn J P;Koppula P R;Stenger H G;Wachs I E .[J].Applied Catalysis B:Environmental,1998,19:103. |
| [118] | Ng K Y S;Gulari E .[J].Journal of Catalysis,1983,92:340. |
| [119] | Knozinger h .[J].Advances in Catalysis,1976,25:184. |
| [120] | Primet M;Pichat P;Mathieu M V i .[J].Journal of Physical Chemistry,1971,75:1216. |
| [121] | Engler B;Koberstein E;Scheubet P .[J].Applied Catalysis,1989,48:71. |
| [122] | Komova L Y;Kovalenko N A;Petkevich T S;Egiazarov Y G .[J].Journal of Applied Spectroscopy,1994,60:487. |
| [123] | Kantcheva M M;Hajiivanov K I;Davydov A A;Budneva A A .[J].Applied Surface Science,1992,55:49. |
| [124] | Hajiivanov K;Klissurski D;Kantcheva M;Davydov A .[J].Journal of the Chemical Society,Faraday Transactions,1991,87:907. |
| [125] | 徐斌;董林;陈懿 .[J].催化学报,1997,18:183. |
| [126] | Zhu HY;Wu Y;Zhao X;Wan HQ;Yang LJ;Hong JM;Yu Q;Dong L;Chen Y;Jian C .Influence of impregnation times on the dispersion of CuO on anatase[J].Journal of molecular catalysis, A. Chemical,2006(1):24-30. |
| [127] | Larsson PO.;Wallenberg LR.;Svensson B.;Andersson A. .COMBUSTION OF CO AND TOLUENE - CHARACTERISATION OF COPPER OXIDE SUPPORTED ON TITANIA AND ACTIVITY COMPARISONS WITH SUPPORTED COBALT, IRON, AND MANGANESE OXIDE[J].Journal of Catalysis,1996(2):279-293. |
| [128] | Li W;Yang R;Kvist K;Regalbuto J R .[J].Energy and Fuels,1997,11:428. |
| [129] | Zhu H Y;Shen M M;Kong Y;Hong J M Hu Y H Liu T D Dong L Chen Y Jian C Liu Z .[J].Journal of Molecular Catalysis A:Chemical,2004,219:155. |
| [130] | Zhu H Y;Shen M M;Wu Y;Li X W Hong J M Liu B Wu X L Dong L Chen Y .[J].Journal of Physical Chemistry B,2005,109:11720. |
| [131] | Najbar M;Mizukami F;Bialas A;Camra J Weselu-cha-Birczyriska A Izutsu H G6ra A .[J].Topics in Catalysis,2000,11-12:131. |
| [132] | Song C Y;Wang C L;Zhu H Y;Wu X C Dong L Chen Y .[J].Catalysis Letters,2008,120:215. |
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