采用盐酸和氢氧化钾对膨润土(BEN)进行改性处理,通过浸渍法制备了改性后膨润土负载的镍催化剂,并对其在二氧化碳甲烷化过程中的催化性能进行了研究.借助BET、XRD、TPR和TPD等测试技术对催化剂进行了表征.结果表明,用碱处理后的膨润土比表面积小于酸处理膨润土的,但以碱处理的膨润土为载体所制备的镍催化剂(Ni/alkali-BEN)具有更高的催化活性和生成甲烷的选择性.CO2-TPD和TPR研究表明,碱处理膨润土后能使镍的还原温度降低,活性中心数量增加,CO2吸附量增大.TPR和XRD测试结果表明,催化剂中易还原的NiO是最主要的镍物种,并且在Ni/alkali-BEN上NiO更多,这可能是其活性高的重要因为.
参考文献
| [1] | Aksoylu A E,Isli A I,Onsaa Z I.Interaction Between Nickel and Molybdenum in Ni-Mo/Al2O3 Catalysts:Ⅲ:Effect of Impregnation Strategy[J].Appl Card A:General,1999,183(2):357-364. |
| [2] | Chang F W,Hsiao T J,Chung S W.Nickel Supported on Rice Husk Ash-activity and Selectivity in CO2 Methanation[J].Appl Catal A:General,1997,164(1/2):225-236. |
| [3] | Michiaki Y,Hiroki H,Katsuhiko A.Effect of Tetragonal ZrO2 on the Catalytic Activity of Ni/ZrO2 Catalyst Prepared from Amorphous Ni-Zr Alloys[J].Catal Commun,2006,7(1):24-28. |
| [4] | JIANG Qi.Methanation of Carbon Dioxide on Supported Iron Catalysts[J].Chinese J Appl Chem,2001,18(7):536-539(in Chinese).江琦.CO2催化加氢甲烷化负载型铁催化剂性能的研究[J].应用化学,2001,18(7):536-539. |
| [5] | SONG Huanling,YANG Jian,ZHAO Jun,et al.Methanation of Carbon Dioxide over a Highly Dispersed Ni/La2O3 Catalyst[J].Chinese J Catal,2010,31(1):21-23(in Chinese).宋焕玲,杨建,赵军,等.CO2在高分散Ni/La2O3催化剂上的甲烷化[J].催化学报,2010,31(1):21-23. |
| [6] | Du G A,Lim S Y,Yang Y H,et al.Methanation of Carbon Dioxide on Ni-incorporated MCM-41 Catalysts:The Influence of Catalyst Pretreatment and Study of Steady-state Reaction[J].J Catal,2007,249(2):370-379. |
| [7] | Kawatra S K,Ripke S J.Developing and Understanding the Bentonite Fiber Bonding Mechanism[J].Miner Eng,2001,14(6):647-659. |
| [8] | Varma R S.Clay and Clay-supported Reagents in Organic Synthesis[J].Tetrahedron,2002,58(7):1235-1255. |
| [9] | Makarand R Gogate,Robert J Davis.Comparative Study of CO and CO2 Hydrogenation over Supported Rh-Fe Catalysts[J].Catal Commun,2010,11(10):901-906. |
| [10] | WANG Chunyan.Study on Acidation Modification of Calci-Bentonite[J].Chem Eng,2002,88(1):11-12(in Chinese).王春艳.钙基膨润土的酸化改性研究[J].化学工程师,2002,88(1):11-12. |
| [11] | QIU Yejun,CHEN Jixiang,ZHANG Jiyan.Effects of MgO Promoter on Properties of Ni/Al2O3 Catalysts for Partial Oxidation of Methane to Syngas[J].J Fuel Chem Technol,2006,34(4):450-455(in Chinese).邱业君,陈吉祥,张继炎.MgO助剂对甲烷部分氧化Ni/Al2O3催化剂结构和性能的影响[J].燃料化学学报,2006,34(4):450-455 |
| [12] | Gao J,Hou Z Y,Guo J Z,et al.Catalytic Conversion of Methane and CO2 to Synthesis Gas over a La2O3-modified SiO2Supported Ni Catalyst in Fluidized-bed Reactor[J].Catal Today,2008,131(1/4):278-284. |
| [13] | ZHANG Yuhong,XIONG Guoxing,SHENG Shishan,et al.Interaction of NiO with γ-Al2O3 Supporter of NiO/γ-Al2O3Catalysts[J].Acta Phys-Chim Sin,1999,15(8):735-741(in Chinese).张玉红,熊国兴,盛世善,等.NiO/γ-Al2O3催化剂中NiO与γ-Al2O3间的相互作用[J].物理化学学报,1999,15(8):735-741. |
| [14] | SONG Yibing,YU Lin,HAO Zhifeng,et al.Relationship Between Preparation Method of Catalyst and Catalytic Activity in the Reaction of Carbon Dioxide Reforming of Methane[J].Chinese J Appl Chem,2001,18(11):903-907(in Chinese).宋一兵,余林,郝志峰,等.CH4、CO2与O2制合成气用Ni-Ce/γ-AlO3催化剂的制备与催化活性的关系[J].应用化学,2001,18(11):903-907. |
| [15] | Diaz A,Acosta D R,Odriozola J A.Characterization of Alkali-Doped Ni/SiO2 Catalysts[J].J Phys Chem B,1997,101(10):1782-1790. |
| [16] | WU Pingxiao.Microstrueture Changes of Montmorillonite After Acid Treatment[J].Modern Chem Ind,2005,25(1):36-38(in Chinese).吴平霄.蒙脱石酸活化与微结构变化关系研究[J].现代化工,2005,25(1):36-38. |
| [17] | YAN Yun,TAN Xiaoyan,LI Song,et al.Study on the Hydroxylation of Benzene to Phenol over Ni-based Catalyst Supported on γ-Al2O3,TiO2,SiO2,NaX[J].Chem Res Appl[J],2008,20(8):1007-1011(in Chinese).严云,谭晓燕,李松,等.几种载体载Ni催化剂上苯直接羟基化制备苯酚的研究[J].化学研究与应用,2008,20(8):1007-1011. |
| [18] | LV Zhijian,QIN Yongning,LI Xiaojie,et al.Study on the Monalayer Dispersion Properties of NiO in Ni/γ-Al2O3Methanation Catalysts[J].Acta Petrolei Sin(Petroleum Processing Section),1995,11(1):20-26(in Chinese).吕志坚,秦永宁,李晓洁,等.镍基甲烷化催化剂的单层分散研究[J].石油学报,1995,11(1):20-26. |
| [19] | ANG Jianxin,LUO Laitao,CHEN Li.Effect of CeO2 on the Performances of CeO2-ZnO Supported Au-Pd Catalysts for Hydrogen Production by Methanol Partial Oxidation[J].Nat Gas Chem Ind,2009,34:30-34(in Chinese).王建鑫,罗来涛,陈丽.CeO2及其含量对Au-Pd/ZnO催化剂甲醇部分氧化制氢性能的影响[J].天然气化工,2009,34:30-34. |
| [20] | Wojcieszak R,Monteverdi S,Mercy M,et al.Nickel Containing MCM-41 and AIMCM-41 Mesoporous Molecular Sieves:Charaeteristies and Activity in the Hydrogenation of Benzene[J].Appl Catal A:General,2004,268(1/2):241-253. |
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%