采用沉淀法制备了Ru/CeO_2氨合成催化剂,并运用N_2物理吸附、X射线衍射、X射线荧光光谱、CO吸附和H2程序升温还原等技术对其进行了表征,考察了沉淀时反应液的并流、反加、正加以及沉积一沉淀对所制备的Ru/CeO_2催化剂氨合成性能的影响.结果表明,不同制备方法所得到的催化剂,其氯残留量和载体的还原性能都存在明显的差别,最终影响了催化剂的氨合成活性,其中采用正加法制备的催化剂上氯残留量少,载体易还原,因而催化活性最高,在10MPa,10 000h~(-1),450℃反应时,NH_3浓度达到11.9%.
The Ru/CeO_2 catalyst was prepared by precipitation methods, including normal precipitation, reverse precipitation, parallel flow precipitation, and deposition-precipitation. The obtained catalysts were characterized by N_2 adsorption-desorption, X-ray diffraction, H_2 temperature-programmed reduction, CO chemisorption, and X-ray fluorescence spectroscopy. The results showed that the ammonia synthesis activity of the Ru/CeO_2 catalyst prepared by normal precipitation was 11.9% at 10 MPa, 10000 h~(-1), and 450 ~C, which was higher than those obtained by other methods. The residual chloride content in this catalyst was much lower and its cerium was easier to be reduced. Thus the activity of the catalyst prepared using normal precipitation was high.
参考文献
[1] | Li L;Zhu Z H;Yan Z F;Lu G Q Rintoul L .[J].Applied Catalysis A:General,2007,320:166. |
[2] | Rossetti I;Mangiarini F;Forni L .[J].Applied Catalysis A:General,2007,323:219. |
[3] | Li Z L;Liang C H;Feng Z C;Ying P L Wang D Z Li C .[J].Journal of Molecular Catalysis A:Chemical,2004,211:103. |
[4] | Kowalczyk Z;Jodzis S;Raróg W;Zielinski J Pielaszek J .[J].Applied Catalysis A:General,1998,173:153. |
[5] | Okal J;Zawadzki M;Kepinski L;Krajczyk L;Tylus W .The use of hydrogen chemisorption for the determination of Ru dispersion in Ru/gamma-alumina catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2007(0):202-209. |
[6] | Kojima R;Enomoto H;Muhler M;Aika K .[J].Applied Catalysis A:General,2003,246:311. |
[7] | Szmigiel D;Raróg-Pilecka W;Miskiewicz E;Glinski M Kielak M Kaszkur Z Kowalczyk Z .[J].Applied Catalysis A:General,2004,273:105. |
[8] | Iwamoto J;Itoh M;Kajita Y;Saito M Machida K .[J].Catalysis Communications,2007,8:941. |
[9] | Murata S;Aika K .[J].Applied Catalysis A:General,1992,82:1. |
[10] | Moggi P;Predieri G;Maione A .[J].Catalysis Letters,2002,79:7. |
[11] | Seetharamulu P;Kumar VS;Padmasri AH;Raju BD;Rao KSR .A highly active nano-Ru catalyst supported on novel Mg-Al hydrotalcite precursor for the synthesis of ammonia[J].Journal of molecular catalysis, A. Chemical,2007(1/2):253-258. |
[12] | Niwa Y;Aika K .[J].Journal of Catalysis,1996,162:138. |
[13] | Niwa Y;Aika K .[J].Chemistry Letters,1996,25:3. |
[14] | Izumi Y;Iwata Y;Aika K .[J].Journal of Physical Chemistry,1996,100:9421. |
[15] | Saito, M;Itoh, M;Iwamoto, J;Li, CY;Machida, K .Synergistic effect of MgO and CeO2 as a support for ruthenium catalysts in ammonia synthesis[J].Catalysis Letters,2006(3/4):107-110. |
[16] | 赵洪雷;郑小明;费金华 .[J].催化学报,1996,17:227. |
[17] | Lee J S;Choi S C .[J].Materials Letters,2004,58:390. |
[18] | Kepinski L;Woicyrz M;Okal J .[J].Journal of the Chemical Society,Faraday Transactions,1995,91:507. |
[19] | Wolcyrz M;Kepinski L .[J].Journal of Solid State Chemistry,1992,99:409. |
[20] | Fu Q;Deng WL;Saltsburg H;Flytzani-Stephanopoulos M .Activity and stability of low-content gold-cerium oxide catalysts for the water-gas shift reaction[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2005(1/2):57-68. |
[21] | Hosokawa S;Kanai H;Utani K;Taniguchi Y I Saito Y Imamura S .[J].Applied Catalysis B:Environmental,2003,45:181. |
[22] | Jacobs G;Chenu E;Patterson P M;Williams L Sparks D Thomas G Davis B H .[J].Applied Catalysis A:General,2004,258:203. |
[23] | Ramaroson E;Tempere J F;Guilleux M F;Vergand F,Roulet H,Dufour G .[J].Journal of the Chemical Society,Faraday Transactions,1992,88:12. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%