采用沉积-沉淀法制备了不同Ce/Zr比的Au/Ce1-xZrxO2(x=0,0.2,0.4,0.6,0.8)催化剂,研究了其催化甲醇完全氧化反应和选择氧化反应中的载体效应.通过X射线衍射、拉曼光谱、X射线光电子能谱、高分辨透射电镜、CO2和NH3程序升温脱附以及CO吸附红外光谱等手段表征了催化剂的结构、组成和酸碱性.结果表明,这些催化剂具有相似的载体粒径和晶相结构、Au担载量、Au粒径和价态以及相似的表面酸碱性等.在甲醇完全氧化和甲醇选择氧化反应中,Au/Ce1-xZrxO2催化剂活性均随载体中Ce/Zr比的减小而降低.与催化剂储氧量,即表面活性氧浓度下降一致.对于甲醇选择氧化反应,甲酸甲酯选择性则随Ce/Zr比减小而升高.这不是由于催化剂表面酸碱性差异所致,而是与催化剂载体中Ce含量降低导致的表面活性氧浓度减小和催化剂的氧化能力减弱密切相关.Au催化剂载体效应本质的认识将有助于为目标氧化反应设计具有更高活性或选择性的催化剂体系.
参考文献
| [1] | Bond G C;Thompson D T .[J].Catalysis Review:Science and Engineering,1999,41:319. |
| [2] | Haruta M;Daté M .[J].Applied Catalysis A:General,2001,222:427. |
| [3] | Choudhary T V;Goodman D W .[J].Topics in Catalysis,2002,21:25. |
| [4] | Kung HH.;Kung MC.;Costello CK. .Supported Au catalysts for low temperature CO oxidation[J].Journal of Catalysis,2003(1/2):425-432. |
| [5] | Stephen A;Hashmi K;Hutchings G J .[J].Angewandte Chemie International Edition,2006,45:7896. |
| [6] | Grzybowska-Swierkosz B .[J].Catalysis Today,2006,112:3. |
| [7] | Kung M C;Davis R J;Kung H H .[J].Journal of Physical Chemistry C,2007,111:11767. |
| [8] | Della Pina C;Falletta E;Prati L;Rossi M .[J].Chemical Society Reviews,2008,37:2077. |
| [9] | Corma A;Garcia H .[J].Chemical Society Reviews,2008,37:2096. |
| [10] | Ma Zh;Dai Sh .[J].Nano Res,2011,4:3. |
| [11] | Wei Y Ch;Liu J;Zhao Zh;Duan A J Jiang G Y .[J].Journal of Catalysis,2012,287:13. |
| [12] | Lopez N;Janssens T V W;Clausen B S;Xu Y Mavrikakis M Bligaard T N(φ)rskov J K .[J].Journal of Catalysis,2004,223:232. |
| [13] | Choudhary TV;Goodman DW .Catalytically active gold: The role of cluster morphology[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2005(1/2):32-36. |
| [14] | Grunwaldt J-D;Maciejewski M;Becker O S;Fabrizioli P Baiker A .[J].Journal of Catalysis,1999,186:458. |
| [15] | Bond G C;Thompson D T .[J].Gold Bulletin,2000,33:41. |
| [16] | Haruta M .[J].Gold Bulletin,2004,37:27. |
| [17] | Weiher N;Bus E;Delannoy L;Louis C;Ramaker DE;Miller JT;van Bokhoven JA .Structure and oxidation state of gold on different supports under various CO oxidation conditions[J].Journal of Catalysis,2006(2):100-107. |
| [18] | Carrettin S;Concepción P;Corma A;Lopez-Nieto J M,Puntes V F .[J].Angewandte Chemie International Edition,2004,43:2538. |
| [19] | Zhang X;Wang H;Xu B Q .[J].Journal of Physical Chemistry B,2005,109:9678. |
| [20] | Schubert M M;Hackenberg S;van Veen A C;Muhler M Plzak V Behm R J .[J].Journal of Catalysis,2001,197:113. |
| [21] | Janssens TVW;Carlsson A;Puig-Molina A;Clausen BS .Relation between nanoscale Au particle structure and activity for CO oxidation on supported gold catalysts[J].Journal of Catalysis,2006(2):108-113. |
| [22] | Kotobuki, M.;Leppelt, R.;Hansgen, D.A.;Widmann, D.;Behm, R.J. .Reactive oxygen on a Au/TiO_2 supported catalyst[J].Journal of Catalysis,2009(1):67-76. |
| [23] | Dobrosz-Gomez I;Kocemba I;Rynkowski J M .[J].Applied Catalysis B:Environmental,2008,83:240. |
| [24] | Dobrosz-Gomez I;Kocemba I;Rynkowski J M .[J].Applied Catalysis B:Environmental,2009,88:83. |
| [25] | Dobrosz-Gomez I;Kocemba I;Rynkowski J M .[J].Catalysis Letters,2009,128:297. |
| [26] | Dobrosz-Gomez I;Gomez-Garcia M A;Rynkowski J M .[J].Polish Journal of Environmental Studies,2009,18:587. |
| [27] | Dobrosz-Gomez, I;Gomez-Garcia, MA;Rynkowski, JM .CO oxidation over Au/CeO2-ZrO2 catalists: The effect of the support composition of the au-support interaction[J].Kinetics and catalysis,2010(6):823-827. |
| [28] | Si R;Zhang Y W;Li Sh J;Lin B X Yan Ch H .[J].Journal of Physical Chemistry B,2004,108:12481. |
| [29] | Zhang H P;Liu H Ch.[J].Journal of Natural Gas Chemistry,2012 |
| [30] | Tatibou(e)t J M .[J].Applied Catalysis A:General,1997,148:213. |
| [31] | Xu B J;Liu X Y;Haubrich J;Madix R J,Friend C M .[J].Angewandte Chemie International Edition,2009,48:4206. |
| [32] | Wittstock A;Zielasek V;Biener J;Friend C M B(a)umer M .[J].Science,2010,327:319. |
| [33] | Han M M;Wang X J;Shen Y N;Tang Ch H Li G Sh Smith R L Jr .[J].JPhys Chem C,2010,114:793. |
| [34] | Liu H;Iglesia E .[J].Journal of Physical Chemistry B,2005,109:2155. |
| [35] | Manzoli M;Boccuzzi F;Chiorino A;Vindigni F Deng W L Flytzani-Stephanopoulos M .[J].Journal of Catalysis,2007,245:308. |
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