采用共沉淀法制各了ZrO_2,Y_(0.1)Zr_(0.9)O_x,Ce_(0.1)Zr_(0.9)O_x和Al_(0.1)Zr_(0.9)O_x系列Zr基载体,并用N_2吸附-脱附和X射线衍射对其进行了表征.再以此为载体,采用浸渍法制备了整体式负载Pd催化剂,催化剂涂层的涂覆量为180g/L左右,Pd含量为1.25%.测定了催化剂上Pd的分散度.在模拟的贫燃天然气汽车尾气中考察了催化剂的活性,并在尾气中有或无SO_2存在的条件F比较了催化剂活性的差异.结果表明,Y~(3+),Ce~(4+)或Al~(3+)改性载体负载的Pd催化剂的耐硫性能明显改善;无论尾气中是否存在SO_2,以Y~(3+)或Al~(3+)改性载体负载的Pd催化剂的活性均明显高于ZrO_2负载体的Pd催化剂.
A series of Zr-based supports such as ZrO_2, Y_(0.1)Zr_(0.9)O_x, Ce_(0.1)Zr_(0.9)O_x, and Al_(0.1)Zr_(0.9)O_x were prepared by a co-precipitation method.The physicochemical properties of the supports were characterized by N_2 adsorption-desorption (the Brunauer-Emmet-Teller method) and X-ray powder diffraction. The Pd-based catalysts were prepared with Pd supported on these supports by the impregnation method. The Pd dispersion on the catalyst surface was characterized by CO chemisorption. The activity of the Pd-based catalysts in a simulated mixture gas from lean-burn natural gas vehicles with and without SO_2 was tested. The results indicated that ZrO_2 modified by Y~(3+), Ce~(4+) or Al~(3+) improved the resistance of the catalysts to sulphur poisoning. The modification of Pd/ZrO_2 with Y~(3+) or AI~(3+) led to more active than the Pd/ZrO_2 catalyst no matter with or without SO_2 in the simulated gas.
参考文献
| [1] | Lampert J K;Kazi M S;Farrauto R J .[J].Applied Catalysis B:Environmental,1997,14:211. |
| [2] | Gelin P;Primet M .[J].Applied Catalysis B:Environmental,2002,39:1. |
| [3] | Janbey A;Clark W;Noordally E;Grimes S Tahir S .[J].CHEMOSPHERE,2003,52:1041. |
| [4] | Burch R.;Loader PK.;Urbano FJ. .METHANE COMBUSTION OVER PALLADIUM CATALYSTS - THE EFFECT OF CARBON DIOXIDE AND WATER ON ACTIVITY[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,1995(1):173-184. |
| [5] | Mowery D L;Graboski M S;Ohno T R;McCormick R L .[J].Applied Catalysis B:Environmental,1999,21:157. |
| [6] | 马中义,徐润,杨成,魏伟,李文怀,孙予罕.不同形态ZrO2的制备及其表面性质研究[J].物理化学学报,2004(10):1221-1225. |
| [7] | 马中义,杨成,董庆年,魏伟,陈建刚,李文怀,孙予罕.不同形态ZrO2负载Co催化剂上CO+H2吸附与反应行为研究[J].高等学校化学学报,2005(05):902-906. |
| [8] | 杨淑梅,邓淑华,黄慧民,余双平.二氧化锆负载催化剂的应用[J].工业催化,2003(10):39-43. |
| [9] | Ohtsuka H;Tabata T;Nakahira T;Masuda M,Hirano T .[P].US 20050002839,2005. |
| [10] | Gelin P;Urfels L;Primet M;Tena E .[J].Catalysis Today,2003,83:45. |
| [11] | Mowery D L;McCormick R L .[J].Applied Catalysis B:Environmental,2001,34:287. |
| [12] | 程新孙,罗来涛,鲁勋.Pd/ZrO2-Al2O3催化剂加氢脱硫性能的研究[J].环境科学研究,2008(01):139-144. |
| [13] | Labaki M.;Siffert S.;Lamonier JF.;Zhilinskaya EA.;Aboukais A. .Total oxidation of propene and toluene in the presence of zirconia doped by copper and yttrium - Role of anionic vacancies[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2003(3):261-271. |
| [14] | Li G R;Li W;Zhang M H;Tao K Y .[J].Catalysis Today,2004,93-95:595. |
| [15] | 李凝,罗来涛,欧阳燕.纳米ZrO2/Al2O3复合载体及Ni/ZrO2/Al2O3催化剂的性能研究[J].催化学报,2005(09):775-779. |
| [16] | 徐占林,王良,赵丽娜,张玉玲,毕颖丽.固体超强酸SO24-/ZrO2-Al2O3催化正丁烷异构化反应研究[J].石油与天然气化工,2006(01):13-15. |
| [17] | Escandon L S;Ordonez S;Vega A;Diez F V .[J].Journal of Hazardous Materials,2008,153:742. |
| [18] | Escandon L S;Ordonez S;Vega A;Diez F V .[J].Chemosphere,2005,58:9. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%