以不同浓度硝酸处理的活性碳(AC)为载体,制备了Co-Zr-La/AC催化剂,并考察了其催化CO加氢制备高碳醇(C6以上)的反应性能.通过Boehm滴定法和N2物理吸附考察了各AC的表面性质,并采用CO化学吸附、程序升温还原和X射线衍射对催化剂进行了表征.结果表明,经硝酸处理后,AC表面酸性基团(如羧基和内酯基)的数量增加,同时催化剂样品上Co和Co2C晶相衍射峰强度也发生变化,从而使催化剂上CO转化率从9.9%提高到65.3%,但醇选择性从62.3%降低到40.5%.当用4.6 mol/L硝酸处理AC时,相应催化剂上的金属态Co和Co2C的比例较为适宜,从而提高了高碳醇在醇中的分布,达40.3%.
参考文献
| [1] | Subramani V;Gangwal S K .[J].Energy & Fuels,2008,22:814. |
| [2] | 王峰云;张慧;辛勤;吴世华 黄维平 戴丽珍 陆大勋 彭少逸 .[J].催化学报,1994,15:79. |
| [3] | 张业,李永旺,孙予罕,钟炳,汤丁亮,徐富春,王水菊.合成低碳醇用超细Mo-Co-K催化剂的XPS研究[J].催化学报,2000(02):109-112. |
| [4] | Zhang H T;Yang X M;Zhou L P;Su Y L Liu Zh M .[J].Journal of Natural Gas Chemistry,2009,18:337. |
| [5] | 苏运来,刘博,裴素朋,王向宇,刘中民.改性Fe-Cu催化剂上由合成气合成酮和醇[J].催化学报,2004(09):683-684. |
| [6] | Yang X M;Yan W;Su Y L;Zhou L P .[J].Fuel Processing Technology,2010,91:1168. |
| [7] | 焦桂萍,丁云杰,朱何俊,李显明,李经伟,董文达,裴彦鹏.活性炭负载钴基催化剂上合成气制混合醇[J].催化学报,2009(08):825-829. |
| [8] | 焦桂萍,丁云杰,朱何俊,李显明,董文达,李经伟,吕元.还原温度对Co-La-Zr/AC催化剂合成气制高碳混合醇性能的影响[J].催化学报,2009(02):92-94. |
| [9] | Jiao G P;Ding Y J;Zhu H J;Li X M Li J W Lin R H Dong W D Gong L F Pei Y P Lü Y .[J].Applied Catalysis A:General,2009,364:137. |
| [10] | Xiong, JM;Ding, YJ;Wang, T;Yan, L;Chen, WM;Zhu, HJ;Lu, Y .The formation of Co2C species in activated carbon supported cobalt-based catalysts and its impact on Fischer-Tropsch reaction[J].Catalysis Letters,2005(3/4):265-269. |
| [11] | Ma W P;Ding Y J;Lin L W .[J].Industrial and Engineering Chemistry Research,2004,43:2391. |
| [12] | Volkova GG.;Plyasova LM.;Naumova MI.;Zaikovskii VI.;Yurieva TM. .Role of the Cu-Co alloy and cobalt carbide in higher alcohol synthesis[J].Journal of molecular catalysis, A. Chemical,2000(1):389-393. |
| [13] | Kang M;Bae Y S;Lee C H .[J].CARBO,2005,43:1512. |
| [14] | Fraga M A;Mendes M J;Jordao E .[J].Journal of Molecular Catalysis A:Chemical,2002,179:243. |
| [15] | Torres G C;Jablonski E L;Baronetti G T;Castro A A de Miguel S R Scelza O A Blanco M D Pena Jimenez M A Fierro J L G .[J].Applied Catalysis A:General,1997,161:213. |
| [16] | Okhlopkova L B;Lisitsyn A S;Likholobov V A;Gurrath M Boehm H P .[J].Applied Catalysis A:General,2000,204:229. |
| [17] | Han W F;Liu H Zh;Zhu H .[J].Catalyst Communication,2007,8:351. |
| [18] | Boehm H P .[J].CARBO,1994,32:759. |
| [19] | Calvo, L;Gilarranz, MA;Casas, JA;Mohedano, AF;Rodriguez, JJ .Effects of support surface composition on the activity and selectivity of Pd/C catalysts in aqueous-phase hydrodechlorination reactions[J].Industrial & Engineering Chemistry Research,2005(17):6661-6667. |
| [20] | 朱虹,韩文锋,柴海芳,刘化章.Ru基氨合成催化剂石墨化炭载体的制备[J].催化学报,2007(03):196-200. |
| [21] | Lopez-Ramon M.V.;Stoeckili F.;Moreno-Castilla C.;Carrasco-Marin F. .On the characterization of acidic and basic surface sites on carbons by various techniques[J].Carbon: An International Journal Sponsored by the American Carbon Society,1999(8):1215-1221. |
| [22] | Li Y H;Lee C W;Gullett B K .[J].Fuel,2003,82:451. |
| [23] | Prado Burguete C;Linares Solano A;Rodriguez Reinoso F;Lecea C S M .[J].Journal of Catalysis,1989,115:98. |
| [24] | 潘崇根,冯国全,李瑛,刘化章.载体活性炭的预处理以及Ru/AC氨合成催化剂的性能[J].化学反应工程与工艺,2010(06):532-538. |
| [25] | 李晓芸,马丁,包信和.不同活性炭上Pt催化剂的分散性及其在甲基环己烷脱氢反应中的催化性能[J].催化学报,2008(03):259-263. |
| [26] | 活性炭表面改性对钌基氨合成催化剂的影响[J].工业催化,2005(10):31-35. |
| [27] | 韩文锋,赵波,霍超,刘化章.活性炭及表面性质对Ru基氨合成催化剂性能的影响[J].催化学报,2004(03):194-198. |
| [28] | 王涛,丁云杰,熊建民,陈维苗,尹红梅,何代平,严丽,林励吾.Zr助剂对Co/AC催化剂催化费-托合成反应性能的影响[J].催化学报,2005(03):178-182. |
| [29] | Guerrero-Ruiz A;Sepulveda-Escribano A;RodriguezRamos I .[J].Applied Catalysis A:General,1994,120:71. |
| [30] | Khodakov A Y;Chu W;Fongarland P .[J].Chemical Reviews,2007,107:1692. |
| [31] | 熊建民,丁云杰,王涛,吕元,朱何俊,罗洪原,林励吾.La2O3助剂对Co/AC催化剂上费-托合成反应性能的影响[J].催化学报,2005(10):874-878. |
| [32] | Coulter KE.;Sault AG. .EFFECTS OF ACTIVATION ON THE SURFACE PROPERTIES OF SILICA-SUPPORTED COBALT CATALYSTS[J].Journal of Catalysis,1995(1):56-64. |
| [33] | Davis B H;Occelli M L.Fischer-Tropsch Synthesis[M].Sasolburg:Elsevier B V,2007:45. |
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%