利用等体积浸渍法制备了氧化硅负载钴催化剂. 通过程序升温还原、氢化学吸附、氧滴定和催化活性评价等手段研究了氧化钡对Co/SiO2的还原性能、钴分散度和颗粒度、分解甲烷活性及其稳定性等的影响. 研究结果表明,氧化钡明显地影响Co/SiO2的还原性能; 添加2%氧化钡提高了Co/SiO2在中温(450℃)条件下的还原度; 氧化钡的还原对Co/SiO2还原的诱导、氧化钡与氧化硅及与氧化钴之间的相互作用是导致Co/SiO2还原性能变化的原因. 氧化钡提高了Co/SiO2的初活性和钴的分散度,降低了钴的颗粒度; 添加0.5%～1.5%氧化钡有利于提高Co/SiO2的稳定性. 钴的分散度和颗粒度影响Co/SiO2的活性和稳定性; 氧化钡的强供电效应也是提高Co/SiO2活性和稳定性的重要因素. 甲烷分解生成的碳物种覆盖了钴活性中心,导致Co/SiO2初活性下降; 但大部分碳物种并不沉积在钴活性中心上,可能形成了碳纤维生长在载体和钴活性中心之间.
参考文献
| [1] | Gueret C.;Billaud F.;Daroux M. .METHANE PYROLYSIS - THERMODYNAMICS[J].Chemical Engineering Science,1997(5):815-827. |
| [2] | Gaudernack B;Lynum S .[J].International Journal of Hydrogen Energy,1999,23(12):1087. |
| [3] | Maitra A M .[J].Applied Catalysis A:General,1993,104(01):11. |
| [4] | Koerts T;Van Santen R A.[J].Journal of the Chemical Society,Chemical Communications,1991(18):1281. |
| [5] | Xu Y;Lin L .[J].Applied Catalysis A:General,1999,188:53. |
| [6] | Fierro J L G;Pena M A;Gomez J P .[J].Applied Catalysis A:General,1996(144):7. |
| [7] | Koerts T;Deelen M J A G;van Santen R A .[J].Journal of Catalysis,1992,138(01):101. |
| [8] | Iglesia E .[J].Applied Catalysis A:General,1997,161:59. |
| [9] | 黄传敬,郑小明,费金华.用不同前驱体制备的Co/SiO2催化剂的结构及其CO2/CH4重整反应性能[J].催化学报,2001(02):138-142. |
| [10] | Zadeh JSM.;Smith KJ. .Kinetics of CH4 decomposition on supported cobalt catalysts[J].Journal of Catalysis,1998(1):115-124. |
| [11] | Coulter KE.;Sault AG. .EFFECTS OF ACTIVATION ON THE SURFACE PROPERTIES OF SILICA-SUPPORTED COBALT CATALYSTS[J].Journal of Catalysis,1995(1):56-64. |
| [12] | Sun S;Tsubaki N;Fujimoto K .[J].Applied Catalysis A:General,2000,202:121. |
| [13] | Steen E;Sewell G S;Makhothe R A;Micklethwaite C,Manstein H,de Lange M,O'Connor C T .[J].Journal of Catalysis,1996,162(02):220. |
| [14] | Guczi L.;Borko L.;Sarma KV. .LOW-TEMPERATURE METHANE ACTIVATION UNDER NONOXIDATIVE CONDITIONS OVER SUPPORTED RUTHENIUM-COBALT BIMETALLIC CATALYSTS[J].Journal of Catalysis,1997(2):495-502. |
| [15] | 吴世华,黄唯平,邱晓航,张守民,郑修成,魏伟.用SMAI法制备的Co/SiO2和Co/La-SiO2催化剂的比较[J].催化学报,2001(05):505-507. |
| [16] | Feller A;Claeys M;Steen E van .[J].Journal of Catalysis,1999,185(01):120. |
| [17] | Kowalczyk Z;Jodzis S;Rarog W;Zielinski J Pielaszek J .[J].Applied Catalysis A:General,1998,173:153. |
| [18] | Choudhary VR.;Mamman AS.;Rajput AM. .NiO alkaline earth oxide catalysts for oxidative methane-to-syngas conversion: Influence of alkaline earth oxide on the surface properties and temperature-programmed reduction/reaction by H-2 and methane[J].Journal of Catalysis,1998(2):576-585. |
| [19] | Reuel R C;Bartholomew C H .[J].Journal of Catalysis,1984,85(01):63. |
| [20] | Bartholomew C H;Farrauto R J .[J].Journal of Catalysis,1976,45(01):41. |
| [21] | Solymosi F;Erdhelyi A;Cserenyi J;Felvegi A .[J].Journal of Catalysis,1994,147(01):272. |
| [22] | Zhang Y;Smith K J.[A].Toronto,2001:85. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%