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采用共沉淀法制备了一系列不同Al_2O_3含量的CeO_2-ZrO_2-Al_2O_3(CZA)氧化物,并用X射线衍射、激光拉曼光谱和N_2吸附.脱附等手段进行了表征.以CZA为载体,采用浸渍法制得钯基催化剂.结果表明,当Al_2O_3含量为80%时,新鲜CZA样品中出现γ-Al_2O_3相.经600℃焙烧后,Al_2O_3在CZA样品中的溶域值略小于80%.经l000℃老化后,CZA样品中Al_2O_3含量为60%时,才开始出现微弱γ-Al_2O_3相,而其他氧化物物相结构稳定.添加Al_2O_3后材料比表面积和储氧量明显增大.随着Al_2O_3含量的增加,CZA样品的储氧量由336.2增至486.2 μmol/g,表现出良好的抗高温老化性能.当Al_2O_3含量为40%时,新鲜催化剂对C_3H_8的起燃温度和完全转化温度分别为238和292℃,同时具有良好的温度特性和较宽的空燃比窗口.

CeO_2-ZrO_2-Al_2O_3 (CZA) samples with different alumina contents were prepared by the co-precipitation method. The CZA samples were characterized by X-ray diffraction (XRD), Raman spectroscopy, N_2 adsorption-desorption, and oxygen storage capacity (OSC) determination. XRD results showed that the samples with Al_2O_3 content lower than 80% could keep the single CeO_2-ZrO_2 cubic fluorite structure after calcination at 600 ℃. However, when the Al_2O_3 content was up to 60%, the γ-Al_2O_3 phase was detected slightly in the aged samples. The results of N_2 adsorption-desorption showed that the specific surface area and the OSC of fresh and aged CZA samples increased with the increase of Al_2O_3 content. The OSC of the aged sample increased from 336.2 to 486.2 μol/g with the increase of Al_2O_3 content from 20% to 80%, indicating that the CZA composite oxide had good thermal stability. A series of Pd/CZA catalyst samples were prepared by impregnation, and the fresh Pd/CZA catalyst with 40% Al_2O_3 had high catalytic activity and broad working-window. Its light-off temperature was 238 ℃, and full conversion temperature was 292 ℃ for C_3H_8.

参考文献

[1] Ohashi M .[J].Shokubai(Catalysts Catal),1987,29:598.
[2] Gandhi H S;Piken A G;Shelef M;Delosh R G .SAE Paper 760201[R].,1976.
[3] Ozawa M;Kimura M;Isogai A .[J].Alloys and Compounds,1993,193:73.
[4] Hori C E;Permana H;Simon Ng K Y;Brenner A More K Rahmoeller K M Belton D .[J].Applied Catalysis B:Environmental,1998,16:105.
[5] Rao Ranga G;Fornasiero P;Di Monte R;Kaspar J Vlaic G Balducci G Meriani S Gubitosa G Cremona A Graziani M .[J].Journal of Catalysis,1996,162:1.
[6] Brezny R;Koranne M M;Egami T;Mamontov E .[P].US20020 132 732,2002.
[7] Colon G;Pijolat M;Valdivieso F;Vidal H,Kaspar J,Finocchio E,Daturi M,Binet C,Lavalley J C,Baker R T,Bernal S .[J].Journal of the Chemical Society,Faraday Transactions,1998,94:3717.
[8] Colon G Valdivieso F;Pijolat M;Baker R T;Calvino J J Bemal S .[J].Catalysis Today,1999,50:271.
[9] 袁书华,王永军,史忠华,赵明,龚茂初,刘忠长,陈启章,陈耀强.满足欧Ⅲ排放标准的压缩天然气汽车中偶催化剂[J].催化学报,2007(05):401-403.
[10] Morikawa A;Suzuki T;Kanazawa T;Kikuta K;Suda A;Shinjo H .A new concept in high performance ceria-zirconia oxygen storage capacity material with Al2O3 as a diffusion barrier[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(3/4):210-221.
[11] Kagpar J;Fornasiero P;Hickey N .[J].Catalysis Today,2003,77:419.
[12] 钟依均,林瑞,罗孟飞.CuO/Ce-Zr-La-O催化剂的表征及CO氧化活性[J].中国稀土学报,2003(02):226-229.
[13] Masui T.;Peng YM.;Machida K.;Adachi GY.;Fujiwara K. .CARBON MONOXIDE OXIDATION CHARACTERISTICS OVER THE AL2O3-SUPPORTED CEO2-ZRO2 CATALYSTS PREPARED BY THE MICROEMULSION METHOD[J].Chemistry Letters,1997(12):1285-1286.
[14] 蔡黎,赵明,皮展,龚茂初,陈耀强.Ce-Zr-La-Al2O3的制备及负载的单Pd三效催化剂[J].催化学报,2008(02):108-112.
[15] Wu XD.;Xu LH.;Weng D. .The thermal stability and catalytic performance of Ce-Zr promoted Rh-Pd/gamma-Al2O3 automotive catalysts[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,2004(1/4):375-383.
[16] Kolli T;Lassi U;Rahkamaa-Tolonen K;Kinnunen TJJ;Keiski RL .The effect of barium on the catalytic behaviour of fresh and aged Pd-Ba-OSC/Al2O3 catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):65-72.
[17] 刘华,史忠华,陈耀强,赵彬,龚茂初.以氨水和碳酸铵为沉淀剂制备氧化铝的对比研究[J].无机化学学报,2004(06):688-692.
[18] Nakano K;Masui T;Adachi G .[J].Journal of Alloys and Compounds,2002,344:342.
[19] 缪建英,蔡俊修.Ce0.5Zr0.5O2固溶体的原位拉曼光谱[J].催化学报,1999(01):25-28.
[20] Sugiura M .[J].Catalysis Surveys From Asia,2003,7:77.
[21] Akira M;Koichi K;Suda A;Shinjo H .[J].Applied Catalysis B:Environmental,2009,88:542.
[22] Zhao M W;Shen M Q;Wang J .[J].Journal of Catalysis,2007,248:258.
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