期刊文献+

ReO_x/ZrO_2催化甲醇一步合成二甲氧基甲烷的研究 被引量:10

One-step synthesis of dimethoxymethane from methanol over ReO_x/ZrO_2
下载PDF
导出
摘要 利用负载型ReOx/ZrO2催化剂,将甲醇选择性氧化并一步合成二甲氧基甲烷。考察了反应时间、反应温度以及铼负载量对反应的影响。并利用N2吸附/脱附、X射线光电子能谱、氨程序升温脱附(NH3-TPD)和氢程序升温还原(H2-TPR)等手段对催化剂进行了表征。结果表明,较高的反应温度有利于提高甲醇的转化率,但对二甲氧基甲烷的选择性不利;催化剂上所负载铼的质量分数对甲醇转化率影响较大,在铼的质量分数为1.64%时转化率达到最大值25.1%;负载于ZrO2上的ReOx具有双功能催化性质:它既可作为氧化中心氧化甲醇,在还原后又可作为酸中心催化醇醛缩合。 The synthesis of dimethoxymethane(DMM) by selective oxidization of methanol over the catalyst rhenium supported on ZrO2 in a fixed-bed reactor was investigated.It was found that higher temperature may promote the conversion of methanol but reduce the selectivity of DMM.The loading of rhenium on the catalyst exhibits a significant influence on methanol conversion and a maximum methanol conversion is obtained at a rhenium loading of 1.64%.XPS,H2-TPR and NH3-TPD suggested that ReOx/ZrO2 acts as a bifunctional catalyst in the reaction: the ReOx supported on ZrO2 is able to oxidize methanol,and then the reduced active sites contribute to the condensation of HCHO and methanol to form DMM.
出处 《燃料化学学报》 EI CAS CSCD 北大核心 2007年第3期334-338,共5页 Journal of Fuel Chemistry and Technology
关键词 二甲氧基甲烷 选择性氧化 铼氧化物 氧化锆 dimethoxymethane selective oxidation methanol rhenium oxide zirconia
  • 相关文献

参考文献9

  • 1王淑娟,陶克毅.合成甲缩醛催化剂和工艺现状[J].辽宁工学院学报,2002,22(5):57-60. 被引量:14
  • 2YUAN Y,LIU H,IMOTO H,SHIDO T,IWASAWA Y.Performance and characterization of a new crystalline SbRe2O6 catalyst for selective oxidation of methanol to methylal[J].J Catal,2000,195(1):51-61.
  • 3YUAN Y,IWASAWA Y.Performance and characterization of supported rhenium oxide catalysts for selective oxidation of methanol to methylal[J].J Phys Chem B,2002,106(17):4441-4449.
  • 4LIU H,IGLESIA E.Selective oxidation of methanol and ethanol on supported ruthenium oxide clusters at low temperatures[J].J Phys Chem B,2005,109(6):2155-2163.
  • 5LIU H,IGLESIA E.Selective one-step synthesis of dimethoxymethane via methanol or dimethyl ether oxidation on H3+nVnMo12-nPO40 keggin structures[J].J Phys Chem B,2003,107(39):10840-10847.
  • 6袁友珠,曹为,蔡启瑞,岩泽康裕.负载型铼催化剂体系与甲醇选择氧化性能的关系[J].高等学校化学学报,2002,23(5):902-905. 被引量:7
  • 7CHAN A S Y,CHEN W,WANG H,ROWE J E,MADEY T E.Methanol reactions over oxygen-modified Re surfaces:Influence of surface structure and oxidation[J].J Phys Chem B.2004,108(38):14643-14651.
  • 8FU Y,ZHU H,SHEN J.Thermal decomposition of dimethoxymethane and dimethyl carbonate catalyzed by solid acids and bases[J].Thermochimica Acta,2005,434(1-2):88-92.
  • 9TATIBOUET J M.Methanol oxidation as a catalytic surface probe[J].Appl Catal A,1997,148(2):213-252.

二级参考文献13

  • 1曾崇余,乔旭.甲缩醛合成催化剂的筛选和工艺条件[J].南京化工学院学报,1993(A07):8-12. 被引量:7
  • 2杨华,项义文.甲醇生产现状及下游产品开发与应用[J].化工商品科技情报,1996,19(1):52-56. 被引量:3
  • 3Butz A., Miehe G., Paulus H. et al.. J. Solid State Chem.[J], 1998, 138: 232-237
  • 4Okal J., Kubicka H.. Appl. Catal. A: General[J], 1998, 171: 351-359
  • 5Okal J., Kepiski K., Krajczyk L. et al.. J. Catal.[J], 1999, 188: 140-153
  • 6Romo C. C., Kühn F. E., Herrmann W. A.. Chem. Rev.[J], 1997, 97: 3 197-3 246
  • 7Gregory S. O., Joachin A., Mahdi M. A. O.. Catal. Today[J], 2000, 55: 317-363
  • 8Espenson J. H.. Chem. Commun.[J], 1999, 479-488
  • 9Kim D. S., Wachs I. E.. J. Catal.[J], 1993, 141: 419-429
  • 10Liu H. C., Gaigneaux E. C., Imoto H. et al.. J. Phys. Chem.[J], 2000, 104: 2 033-2 043

共引文献18

同被引文献207

引证文献10

二级引证文献51

相关作者

内容加载中请稍等...

相关机构

内容加载中请稍等...

相关主题

内容加载中请稍等...

浏览历史

内容加载中请稍等...
;
使用帮助 返回顶部