采用共沉淀法制备了未改性的和Ca掺杂的CeO2-ZrO2-Al2O3样品,进一步用浸渍法制备了Pd/CeO2-ZrO2-Al2O3(Pd/CZA)和Pd/CeO2-ZrO2-Al2O3-CaO (Pd/CZACa)催化剂.运用X射线衍射、N2吸附-脱附、储氧量测定、CO化学吸附、NH3程序升温脱附、CO2程序升温脱附、H2程序升温还原和X射线光电子能谱对催化剂进行了表征,并考察了其催化甲醇裂解反应活性.结果表明,Ca的添加使载体酸性位中毒,弱碱中心数目增加,从而影响了催化剂上吸附物种的吸附-脱附平衡过程；同时,使得金属和载体问相互作用增强,增加了Pd周围的电子密度,使Pd保持在部分氧化状态Pdδ+(0＜δ＜2),进而提高了甲醇催化裂解反应的活性,使甲醇完全裂解温度降低了34℃.
参考文献
| [1] | Aboul-Fotouh S M K;Aboul-Gheit N A K;Hassan M M I .[J].催化学报,2011,32:412. |
| [2] | Liu Y Y;Hayakawa T;Ishii T;Kumagai M Yasuda H Suzuki K Hamakawa S Murata K .[J].Applied Catalysis A:General,2001,210:301. |
| [3] | Kapoor M P;Ichihashi Y;Kuraoka K;Shen W J Matsumura Y .[J].Catalysis Letters,2003,88:1. |
| [4] | Sun K P;Lu W W;Wang M;Xu X L .[J].Applied Catalysis A:General,2004,268:107. |
| [5] | Wang H R;Chen Y Q;Zhang Q L;Zhu Q Ch Gong M Ch Zhao M .[J].Journal of Natural Gas Chemistry,2009,18:211. |
| [6] | Cheng W H .[J].Accounts of Chemical Research,1999,32:685. |
| [7] | Matsumura Y;Shen W J .[J].Topics in Catalysis,2003,22:271. |
| [8] | Sakai T;Yamaguchi I;Asano M;Ayusawa T,Kim Y K .SAE paper,JPN 871169[R].,1987. |
| [9] | 杨成,任杰,孙予罕.CeO2和La2O3改性Pd/γ-Al2O3甲醇低温分解催化剂的研究Ⅰ.CeO2改性Pd/γ-Al2O3催化剂的结构和性能[J].催化学报,2001(03):283-286. |
| [10] | Kapoor M P;Ichihashi Y;Nakamori T;Matsumura Y .[J].Journal of Molecular Catalysis A:Chemical,2004,213:251. |
| [11] | Zhao M W;Shen M Q;Wen X M;Wang J .[J].Journal of Alloys and Compounds,2008,457:578. |
| [12] | Fernández-García M;Martinez-Arias A;Guerrero-Ruiz A;Conesa J C Soria J .[J].Journal of Catalysis,2002,211:326. |
| [13] | Kouzu M;Kasuno T;Tajika M;Sugimoto Y Yamanaka S Hidaka J .[J].Fuel,2008,87:2798. |
| [14] | Vujicic D;Comic D;Zarubica A;Micic R Boskovic G .[J].Fuel,2010,89:2054. |
| [15] | Zhao M;Yang X Sh;Church T L;Harris A T .[J].International Journal of Hydrogen Energy,2011,36:421. |
| [16] | Scire S.;Maggiore R.;Minico S.;Galvagno S.;Crisafulli C. .Effect of the acid-base properties of Pd-Ca/Al2O3 catalysts on the selective hydrogenation of phenol to cyclohexanone: FT-IR and TPD characterization[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,1998(4):311-320. |
| [17] | Yue B H;Zhou R X;Zheng X M;Lu W C .[J].Fuel Processing Technology,2008,89:728. |
| [18] | Cabilla G C;Bonivardi A L;Baltanas M A .[J].Journal of Catalysis,2001,201:213. |
| [19] | Cai L;Wang K C;Zhao M;Gong M C Chen Y Q .[J].Acta Physico-Chimica Sinica,2009,25:859. |
| [20] | 龙恩艳,王云,张晓玉,李移乐,龚茂初,陈耀强.Zr基载体负载Pd催化剂用于贫燃天然气汽车尾气净化[J].催化学报,2010(03):313-316. |
| [21] | 赵明,王海蓉,陈山虎,姚艳玲,龚茂初,陈耀强.CeO_（2-）ZrO（2-）Al_2O_3的制备及其负载钯三效催化剂的催化性能[J].催化学报,2010(04):429-434. |
| [22] | 李红梅,周菊发,祝清超,曾少华,魏振玲,陈耀强,龚茂初.共沉淀法制备的CeO_2-ZrO_2-Al_2O_3材料及性能[J].高等学校化学学报,2009(12):2484-2486. |
| [23] | 杨春雁,杨卫亚,凌凤香,范峰.负载型金属催化剂表面金属分散度的测定[J].化工进展,2010(08):1468-1473,1501. |
| [24] | 姚艳玲,何胜楠,史忠华,龚茂初,陈耀强.BaO含量对Ba改性Al2O3及其负载的Pt-Rh密偶催化剂性能的影响[J].催化学报,2011(03):502-507. |
| [25] | 储伟.催化剂工程[M].成都:四川大学出版社,2006:245. |
| [26] | Jin R B;Liu Y;Wu Zh B;Wang H Q Gu T T .[J].Chemosphere,2010,78:1160. |
| [27] | Mhamdi M;Khaddar-Zine S;Ghorbel A .[J].Applied Catalysis A:General,2009,357:42. |
| [28] | Neri G;Visco A M;Donato A;Milone C Malentacchi M Gubitosa G .[J].Applied Catalysis A:General,1994,110:49. |
| [29] | Fuentes S;Bogdanchikova N;Avalos-Borja M;Boronin A Farias M H Diaz G Cortes A G Barrera A .[J].Catalysis Today,2000,55:301. |
| [30] | Barrera A.;Bosch P.;Lara VH.;Fuentes S.;Viniegra M. .Pd/Al2O3-La2O3 catalysts prepared by sol-gel: characterization and catalytic activity in the NO reduction by H-2[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2001(2):97-111. |
| [31] | Kili K;Hilaire L;Normand F L .[J].Physical Chemistry Chemical Physics,1999,1:1623. |
| [32] | Briggs D;Seah M.Practical Surface Analysis[M].New York:wiley,1990:243. |
| [33] | Yoshida H;Yazawa Y;Hattori T .[J].Catalysis Today,2003,87:19. |
| [34] | Yoshida H;Nakajima T;Yazawa Y;Hattori T .Support effect on methane combustion over palladium catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(1/2):70-79. |
| [35] | Yazawa Y;Yoshida H;Takagi N;Komai S Satsuma A Hattori T .[J].Journal of Catalysis,1999,187:15. |
| [36] | Yazawa Y;Yoshida H;Takagi N;Kagi N Komai S Satsuma A Murakami Y Hattori T .[J].Studies in Surface Science and Catalysis,2000,130:2189. |
| [37] | Yoshida H;Tsuruta T;Yazawa Y;Hattori T .[J].Applied Catalysis A:General,2007,325:50. |
| [38] | Schmitz A D;Eyman D P;Gloer K B .[J].Energy & Fuels,1994,8:729. |
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