探究负载金属氧化物的结构是确立催化剂结构和催化性能之间相互关系的首要条件。在众多表征技术中,多波长拉曼光谱结合了共振拉曼和由不同波长激发的非共振拉曼,不仅在识别负载金属氧化物团簇的结构,而且在定量方面已经成为强有力的工具。本文以两个负载氧化钒体系(VOx/SiO2, VOx/CeO2)为例,阐述了如何利用该技术研究活性氧化物团簇的多相结构,并理解氧化物团簇和载体之间复杂的相互作用。由多波长拉曼光谱得到的定性和定量信息能为设计更有效的负载金属氧化物催化剂提供基本的依据。
Revealing the structure of supported metal oxide catalysts is a prerequisite for establishing the structure-catalysis relationship. Among a variety of characterization techniques, multi-wavelength Raman spectroscopy, combining resonance Raman and non-resonance Raman with different excita-tion wavelengths, has recently emerged as a particularly powerful tool in not only identifying but also quantifying the structure of supported metal oxide clusters. In this review, we make use of two supported vanadia systems, VOx/SiO2 and VOx/CeO2, as examples to showcase how one can employ this technique to investigate the heterogeneous structure of active oxide clusters and to understand the complex interaction between the oxide clusters and the support. The qualitative and quantita-tive structural information gained from the multi-wavelength Raman spectroscopy can be utilized to provide fundamental insights for designing more efficient supported metal oxide catalysts.
参考文献
[1] | Banares M A;Wach I E .[J].J Raman Spectr,2002,33:359. |
[2] | Wachs I E;Roberts C A .[J].CHEMICAL SOCIETY REVIEWS,2010,39:5002. |
[3] | Banares M A;Mestl G .[J].ADVANCES IN CATALYSIS,2009,52:43. |
[4] | Stavitski E;Weckhuysen B M .[J].CHEMICAL SOCIETY REVIEWS,2010,39:4615. |
[5] | Kim H;Kosuda K M;Van Duyne R P;Stair P C .[J].CHEMICAL SOCIETY REVIEWS,2010,39:4820. |
[6] | Wu Z L;Kim H S;Stair P C;Rugmini S Jackson S D .[J].Journal of Physical Chemistry B,2005,109:2793. |
[7] | Kim H S;Zygmunt S A;Stair P C;Zapol P Curtiss L A .[J].J Phys Chem C,2009,113:8836. |
[8] | Kim H S;Stair P C .[J].Journal of Physical Chemistry A,2009,113:4346. |
[9] | Xiong G;Feng Z C;Li J;Yang Q H Ying P L Xin Q Li C .[J].Journal of Physical Chemistry B,2000,104:3581. |
[10] | Li M J;Feng Z H;Xiong G;Ying P L Xin Q Li C .[J].Journal of Physical Chemistry B,2001,105:8107. |
[11] | Li C. .UV Resonance Raman Spectroscopic Identification of Titanium Atioms in the Framework of TS-1 Zeolite[J].Angewandte Chemie International Edition,1999(15):2220-2222. |
[12] | Stair P C .[J].ADVANCES IN CATALYSIS,2007,51:75. |
[13] | Fan F T;Feng Z C;Li C .[J].Accounts of Chemical Research,2010,43:378. |
[14] | Wang J Y;Li G N;Ju X H;Xia H A Fan F T Wang J H Feng Z C Li C .[J].Journal of Catalysis,2013,301:77. |
[15] | Guo, Q.;Sun, K.;Feng, Z.;Li, G.;Guo, M.;Fan, F.;Li, C. .A thorough investigation of the active titanium species in TS-1 zeolite by in situ UV resonance raman spectroscopy[J].Chemistry: A European journal,2012(43):13854-13860. |
[16] | Jin S Q;Guo M L;Fan F T;Yang J X Zhang Y Huang B K Feng Z C Li C .[J].J Raman Spectr,2013,44:266. |
[17] | Kim H;Ferguson G A;Cheng L;Zygmunt S A Stair P C Curtiss L A .[J].J Phys Chem C,2012,116:2927. |
[18] | López I;Ertem M Z;Maji S;Benet-Buchholz J Keidel A Kuhlmann U Hildebrandt P Cramer C J Batista V S Llobet A .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2014,53:205. |
[19] | Woertink J S;Smeets P J;Groothaert M H;Vance M A Sels B F Schoonheydt R A Solomon E I .[J].Proceedings of the National Academy of Sciences(USA),2009,106:18908. |
[20] | Nitsche, D.;Hess, C. .In situ diagnostics of catalytic materials using tunable confocal Raman spectroscopy[J].Journal of Raman Spectroscopy: An International Journal for Original Work in All Aspects of Raman Spectroscopy, Including Higher Order Processes, and Also Brillouin- and Rayleigh Scattering,2013(12):1733-1738. |
[21] | Wu Z L;Kim H-S;Stair P C;Hargraves J S J,Jackson S D.Metal Oxide Catalysis[M].,2008:177. |
[22] | Launay H;Loridant S;Pigamo A;Dubois J L Millet J M M .[J].Journal of Catalysis,2007,246:390. |
[23] | Sun Q;Jehng J M;Hu H C;Herman R G Wachs I E Klie K .[J].Journal of Catalysis,1997,165:91. |
[24] | Banares MA.;Agullo-Rueda F.;Correa-Bueno JM.;Fierro JLG.;Cardoso JH. .Dynamic states of V-oxide species: reducibility and performance for methane oxidation on V2O5/SiO2 catalysts as a function of coverage[J].Catalysis Letters,2000(2/4):191-196. |
[25] | Weckhuysen B M;Kelle D E .[J].Catalysis Today,2003,78:25. |
[26] | Wachs, I.E. .Catalysis science of supported vanadium oxide catalysts[J].Dalton transactions: An international journal of inorganic chemistry,2013(33):11762-11769. |
[27] | Wu Z L;Dai S;Overbury S H .[J].J Phys Chem C,2010,114:412. |
[28] | Wu Z L;Li M J;Overbury S H .[J].ChemCatChem,2012,4:1653. |
[29] | Wu Z L;Schwartz V;Li M;Rondinone A J Overbury S H .[J].J Phys Chem Lett,2012,3:1517. |
[30] | Wu Z L;Rondinone A J;Ivanov I N;Overbury S H .[J].J Phys Chem C,2011,115:25368. |
[31] | Gao X T;Bare S R;Weckhuysen B M;Wachs I E .[J].Journal of Physical Chemistry B,1998,102:10842. |
[32] | 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. |
[33] | Wang CB.;Wachs IE.;Deo G. .Characterization of vanadia sites in V-silicalite, vanadia-silica cogel, and silica-supported vanadia catalysts: X-ray powder diffraction, Raman spectroscopy, solid-state V-51 NMR, temperature-programmed reduction, and methanol oxidation studies[J].Journal of Catalysis,1998(2):640-648. |
[34] | Jehng J M;Hu H C;Gao X T;Wachs I E .[J].Catalysis Today,1996,28:335. |
[35] | Das N;Eckert H;Hu H C;Wachs I E Walzer J F Feher F J .[J].Journal of Physical Chemistry,1993,97:8240. |
[36] | Lee E L;Wachs I E .[J].J Phys Chem C,2007,111:14410. |
[37] | Dinse A;Ozarowski A;Hess C;Schomacker R Dinse K P .[J].J Phys Chem C,2008,112:17664. |
[38] | Wachs I E;Weckhuysen B M .[J].Applied Catalysis A:General,1997,157:67. |
[39] | Keller D E;Koningsberger D C;Weckhuysen B M .[J].Journal of Physical Chemistry B,2006,110:14313. |
[40] | Liu Y M;Cao Y;Yi N;Feng W L Dai W L Yan S R He H Y Fan K N .[J].Journal of Catalysis,2004,224:417. |
[41] | Khodakov A;Olthof B;Bell A T;Iglesia E .[J].Journal of Catalysis,1999,181:205. |
[42] | Magg N;Immaraporn B;Giorgi JB;Schroeder T;Baumer M;Dobler J;Wu ZL;Kondratenko E;Cherian M;Baerns M;Stair PC;Sauer J;Freund HJ .Vibrational spectra of alumina- and silica-supported vanadia revisited: An experimental and theoretical model catalyst study[J].Journal of Catalysis,2004(1):88-100. |
[43] | Gijzeman OLJ;van Lingen JNJ;van Lenthe JH;Tinnemans SJ;Keller DE;Weckhuysen BM .A new model for the molecular structure of supported vanadium oxide catalysts[J].Chemical Physics Letters,2004(1/3):277-281. |
[44] | van Lingen J N J;Gijzerman O L J;Weckhuysen B M;van Lenthe J H .[J].Journal of Catalysis,2006,239:34. |
[45] | Keller D E;Visser T;Soulimani F;Koningsberger D C Weckhuysen B M .[J].Vib Spectr,2007,43:140. |
[46] | Moisii C;van de Burgt L J;Stiegman A E .[J].CHEMISTRY OF MATERIALS,2008,20:3927. |
[47] | Moisii C;Curran MD;van de Burgt LJ;Stiegman AE .Raman spectroscopy of discrete silica supported vanadium oxide: assignment of fundamental stretching modes[J].Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology,2005(34):3519-3524. |
[48] | Lee EL;Wachs IE .In situ Raman spectroscopy of SiO2-supported transition metal oxide catalysts: An isotopic O-18-O-16 exchange study[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2008(16):6487-6498. |
[49] | Guimond S;Abu Haija M;Kaya S;Lu J Weissenrieder J Shaikhutdinov S Kuhlenbeck H Freund H J Dobler J Sauer J .[J].Topics in Catalysis,2006,38:117. |
[50] | Lewandowska A E;Banares M A;Tielens F;Che M Dzwigaj S .[J].J Phys Chem C,2010,114:19771. |
[51] | Chlosta R;Tzolova-Muller G;Schlogl R;Hess C .[J].Catal Sci Technol,2011,1:1175. |
[52] | van Lingen JNJ;Gijzeman OLJ;Havenith RWA;van Lenthe JH .Determining the structure of silica-supported monomeric vanadium oxide catalysts based on synthesis method and spectral data from theoretical calculations[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2007(19):7071-7077. |
[53] | Islam M M;Costa D;Calatayud M;Tielens F .[J].J Phys Chem C,2009,113:10740. |
[54] | Ohde C;Brandt M;Limberg C;Doebler J;Ziemer B;Sauer J .V2O5/SiO2 surface inspired, silsesquioxane-derived oxovanadium complexes and their properties[J].Dalton transactions: An international journal of inorganic chemistry,2008(3):326-331. |
[55] | Todorova T K;Dobler J;Sierka M;Sauer J .[J].J Phys Chem C,2009,113:8336. |
[56] | D?bler J;Pritzsche M;Sauer J .[J].J Phys Chem C,2009,113:12454. |
[57] | Burcham L J;Deo G;Gao X T;Wachs I E .[J].Topics in Catalysis,2000,11:85. |
[58] | Keller D E;de Groot F M F;Koningsberger D C;Weckhuysen B M .[J].Journal of Physical Chemistry B,2005,109:10223. |
[59] | Molinari, J.E.;Wachs, I.E. .Presence of surface vanadium peroxo-oxo umbrella structures in supported vanadium oxide catalysts: Fact or fiction?[J].Journal of the American Chemical Society,2010(36):12559-12561. |
[60] | Cavalleri, M.;Hermann, K.;Knop-Gericke, A.;H?vecker, M.;Herbert, R.;Hess, C.;Oestereich, A.;D?bler, J.;Schl?gl, R. .Analysis of silica-supported vanadia by X-ray absorption spectroscopy: Combined theoretical and experimental studies[J].Journal of Catalysis,2009(2):215-223. |
[61] | H?vecker M;Cavalleri M;Herbert R;Follath R Knop-Gericke A Hess C Hermann K Schl?gl R .[J].PHYSICA STATUS SOLIDI B-BASIC RESEARCH,2009,246:1459. |
[62] | Bulanek R;Capek L;Setnicka M;Cicmanec P .[J].J Phys Chem C,2011,115:12430. |
[63] | Galeener F L;Mikkelsen J C .[J].Physical Review B:Condensed Matter,1981,23:5527. |
[64] | Gao X T;Wachs I E .[J].Journal of Physical Chemistry B,2000,104:1261. |
[65] | Tian H J;Ross E I;Wachs I E .[J].Journal of Physical Chemistry B,2006,110:9593. |
[66] | Albrecht A C .[J].Journal of Chemical Physics,1961,34:1476. |
[67] | Koningstein J A .[J].J Mol Spectr,1968,28:309. |
[68] | Tang J;Albrecht A C;Szymanski H A.Raman Spectroscopy[M].New York:Plenum,1970:33. |
[69] | Clark R J H;Stewart B.Inorganic Chemistry and Spectroscopy[M].Berlin:Springer Berlin Heidelberg,1979:36:1. |
[70] | Long D A.The Raman Effect:A Unified Treatment of the Theory of Raman Scattering by Molecules[M].New York:Wiley,2002:1. |
[71] | Cotton F A;Wing R M .[J].Inorganic Chemistry,1965,4:867. |
[72] | Wu Z L;Zhang C;Stair P C .[J].Catalysis Today,2006,113:40. |
[73] | Wu Z;Stair P C;Rugmini S;Jackson S D .[J].J Phys Chem C,2007,111:16460. |
[74] | Gao X T;Banares M A;Wachs I E .[J].Journal of Catalysis,1999,188:325. |
[75] | Daniell W;Ponchel A;Kuba S;Anderle F Weingand T Gregory D H Knoezinger H .[J].Topics in Catalysis,2002,20:65. |
[76] | Martinez-Huerta M V;Coronado J M;Fernandez-Garcia M;Iglesi-as-Juez A Deo G Fierro J L G Banares M A .[J].Journal of Catalysis,2004,225:240. |
[77] | Martinez-Huerta M V;Deo G;Fierro J L G;Banares M A .[J].J Phys Chem C,2007,111:18708. |
[78] | Martinez-Huerta M V;Deo G;Fierro J L G;Banares M A .[J].J Phys Chem C,2008,112:11441. |
[79] | Ganduglia-Pirovano, MV;Popa, C;Sauer, J;Abbott, H;Uhl, A;Baron, M;Stacchiola, D;Bondarchuk, O;Shaikhutdinov, S;Freund, HJ .Role of Ceria in Oxidative Dehydrogenation on Supported Vanadia Catalysts[J].Journal of the American Chemical Society,2010(7):2345-2349. |
[80] | Taylor M N;Carley A F;Davies T E;Taylor S H .[J].Topics in Catalysis,2009,52:1660. |
[81] | Abbott, H.L.;Uhl, A.;Baron, M.;Lei, Y.;Meyer, R.J.;Stacchiola, D.J.;Bondarchuk, O.;Shaikhutdinov, S.;Freund, H.J. .Relating methanol oxidation to the structure of ceria-supported vanadia monolayer catalysts[J].Journal of Catalysis,2010(1):82-91. |
[82] | Feng T;Vohs J M .[J].Journal of Catalysis,2004,221:619. |
[83] | Wong G S;Concepcion M R;Vohs J M .[J].Journal of Physical Chemistry B,2002,106:6451. |
[84] | Wu Y N;Guo M;Chen F;Luo M F .[J].ACTA PHYSICO-CHIMICA SINICA,2010,26:2417. |
[85] | Matta J.;Courcot D.;Abi-Aad E.;Aboukais A. .Identification of vanadium oxide species and trapped single electrons in interaction with the CeVO4 phase in vanadium-cerium oxide systems. V-51 MAS NMR, EPR, Raman, and thermal analysis studies[J].Chemistry of Materials,2002(10):4118-4125. |
[86] | Jehng J M;Deo G;Weckhuysen B M;Wachs I E .[J].Journal of Molecular Catalysis A:Chemical,1996,110:41. |
[87] | Wachs IE.;Deo G.;Weckhuysen BM.;Guliants VV.;Benziger JB. Sundaresan S.;Jehng JM. .FUNDAMENTAL STUDIES OF BUTANE OXIDATION OVER MODEL-SUPPORTED VANADIUM OXIDE CATALYSTS - MOLECULAR STRUCTURE-REACTIVITY RELATIONSHIPS[J].Journal of Catalysis,1997(1):75-88. |
[88] | Reddy B M;Khan A;Yamada Y;Kobayashi T Loridant S Volta J C .[J].Journal of Physical Chemistry B,2003,107:5162. |
[89] | Banares M A;Martinez-Huerta M V;Gao X T;Wachs I E Fierro J L G .[J].Studies in surface science and catalysis,2000,130:3125. |
[90] | Burcham L J;Wachs I E .[J].Catalysis Today,1999,49:467. |
[91] | Baron M;Abbott H;Bondarchuk O;Stacchiola D Uhl A Shaikhutdinov S Freund H J Popa C Ganduglia-Pirovano M V Sauer J .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2009,48:8006. |
[92] | Popa C;Ganduglia-Pirovano M V;Sauer J .[J].J Phys Chem C,2011,115:7399. |
[93] | Shapovalov V;Metiu H .VOx (x=1-4) submonolayers supported on rutile TiO2(110) and CeO2(111) surfaces: The structure, the charge of the atoms, the XPS spectrum, and the equilibrium composition in the presence of oxygen[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2007(38):14179-14188. |
[94] | Qiao Z A;Wu Z L;Dai S .[J].ChemSusChem,2013,6:1821. |
[95] | Wu Z L;Li M J;Howe J;Meyer H M Overbury S H .[J].LANGMUIR,2010,26:16595. |
[96] | Taniguchi T;Watanabe T;Sugiyama N;Subramani A K Wagata H Matsushita N Yoshimura M .[J].J Phys Chem C,2009,113:19789. |
[97] | Guo, M.;Lu, J.;Wu, Y.;Wang, Y.;Luo, M. .UV and visible Raman studies of oxygen vacancies in rare-earth-doped ceria[J].Langmuir: The ACS Journal of Surfaces and Colloids,2011(7):3872-3877. |
[98] | Li, L.;Chen, F.;Lu, J.-Q.;Luo, M.-F. .Study of defect sites in ce1-xmxo2-δ (x = 0.2) solid solutions using raman spectroscopy[J].The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory,2011(27):7972-7977. |
[99] | Li L;Hu G S;Lu J Q;Luo M F .[J].ACTA PHYSICO-CHIMICA SINICA,2012,28:1012. |
[100] | Zhou K B;Wang X;Sun X M;Peng Q Li Y D .[J].Journal of Catalysis,2005,229:206. |
[101] | Mai H X;Sun L D;Zhang Y W;Si R Feng W Zhang H P Liu H C Yan C H .[J].Journal of Physical Chemistry B,2005,109:24380. |
[102] | Trovarelli A .[J].CATALYSIS REVIEWS-SCIENCE AND ENGINEERING,1996,38:439. |
[103] | Pushkarev V V;Kovalchuk V I;d'Itri J L .[J].Journal of Physical Chemistry B,2004,108:5341. |
[104] | Li C;Domen K;Maruya K;Onishi T .[J].Journal of the American Chemical Society,1989,111:7683. |
[105] | Banares M A .[J].Advanced Materials,2011,23:5293. |
[106] | Nolan M;Fearon JE;Watson GW .Oxygen vacancy formation and migration in ceria[J].Solid state ionics,2006(35/36):3069-3074. |
[107] | Nolan M;Grigoleit S;Sayle DC;Parker SC;Watson GW .Density functional theory studies of the structure and electronic structure of pure and defective low index surfaces of ceria[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,2005(1/3):217-229. |
[108] | Wu Z L;Li M J;Overbury S H .[J].Journal of Catalysis,2012,285:61. |
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