采用超临界甲醇处理活性炭,水浸渍制备负载钌炭催化剂,用N2物理吸附、Boehm滴定、X光电子能谱(XPS)和程序升温还原(TPR)等测试技术研究了超临界甲醇处理对活性炭表面结构及表面基团相对含量的影响,并以葡萄糖加氢生产山梨醇为模型反应对钌基催化剂的性能进行了评价.研究结果表明,超临界甲醇处理活性炭,活性炭的孔结构性能变化不大,但可有效降低活性炭表面含氧酸性基团的含量,使催化剂的还原温度升高,增强了载体和活性组分间的相互作用,有效的提高了钌的分散度,从而提高所负载催化剂的催化活性.在实验范围内,当超临界甲醇的温度为300℃,处理时间为12 h时,在4.0 MPa、120℃、葡萄糖的质量分数为50％的反应条件下,催化剂的反应速率(按Ru单位质量计)达到了118.65 mmol/(min·g),是未处理活性炭的1.96倍.
参考文献
| [1] | Rodriguez Reinoso F.The Role of Carbon Materials in Heterogeneous Catalysis[J].Carbon,1998,36(3):159-175. |
| [2] | Figueiredo J L,Pereira M F R,Freitas M M A,et al.Modification of The Surface Chemistry of Activated Carbons[J].Carbon,1999,37(9):1379-1389. |
| [3] | Pierre Gallezot,Nathalie Nicolaus,Guy Fleche,et al.Glucose Hydrogenation on Ruthenium Catalysts in A Trickle-Bed Reactor[J].J Catal,1998,180(1):51-55. |
| [4] | Hoffer B W,Crezee E,Mooijman P R M,et al.Carbon Supported Ru Catalysts as Promising Alternative for Raney-type Ni in The Selective Hydrogenation of D-glucose[J].Catal Today,2003,35:79-83. |
| [5] | Aksoylu A E,Freitas M M A,Figueiredo J L,et al.Bimetallic Pt-Sn Catalysts Supported on Activated Carbon:The Effects of Support Modification and Impregation Strategy[J].Appl Catal A:General,2000,192(1):29-42. |
| [6] | ZHENG Xiaoling,FU Wujun,YU Yubin,et al.Effect of Microwave Treatment of Activated Carbon Support on Catalytic Performance of Ru/C for Ammonia Synthesis[J].Chinese J Catal,2002,23(6):562-566(in Chinese).郑晓玲,傅武俊,俞裕斌,等.活性炭载体的微波处理对氨合成催化剂Ru/C催化性能的影响[J].催化学报,2002,23(6):562-566. |
| [7] | YU Fengwen,JI Jianbing,HUO Chao,et al.Effect of Ultrasonic Frequency on Structure of Activated Carbon and Activity of Ru/AC Catalyst for Ammonia Synthesis[J].Chinese J Catal,2006,27(6):511-515(in Chinese).于风文,计建炳,霍超,等.超声频率对活性炭结构及钌/活性炭氨合成催化剂催化活性的影响[J].催化学报,2006,27(6):511-515. |
| [8] | CHEN Hejing.Study on Pretreatment Method of Ru/C Catalysts[D].Zhengzhou:Zhengzhou University,2007 (in Chinese).陈何敬.Ru/C催化剂的处理方法研究[D].郑州:郑州大学,2007. |
| [9] | Zhang Y,Erkey C.Preparation of Supported Metallic Nanoparticles Using Supercritical Fluids:A Review[J].J Supercrit Fluids,2006,38:252-267. |
| [10] | Can Erkey.Preparation of Metallic Supported Nanoparticles and Films Using Supercritical Fluid Deposition[J].J Supercrit Fluids,2009,47:517-522. |
| [11] | FAN Haijuan,XU Qun,CAO Yonxia,et al.Preparation of Porous Alumina Material with Template Method in Supercritical CO2[J].Chinese J Appl Chem,2007,24(1):17-20(in Chinese).范海娟,许群,曹艳霞,等.超临界CO2中模板法制备氧化铝多孔材料[J].应用化学,2007,24(1):17-20. |
| [12] | Atamny F,Blocker J.Surface Chemistry of Carbon:Activation of Molecular Oxygen[J].Mol Phys,1992,76(4):851-886. |
| [13] | Reis M J,Botelho A M,Do Rego,et al.An XPS Study of the Fibre-Matrix Interface Using Sized Carbon Fibres as A Model[J].J Mater Sci,1995,30(1):118-126. |
| [14] | Goloma F,Sepulveda-Escribano A,Fierro J L G,et al.Gas Phase Hydrogenation of Crotonaldehyde over P/Activated Carbon Catalysts,Influence of the Oxygen Surface Groups on The Support[J].Appl Catal A:General,1997,150:165-183. |
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%