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ReOxZrO2催化甲醇一步合成二甲氧基甲烷的研究
引用本文:曹虎,郑岩,马珺,李军平,赵宁,王秀芝,魏伟,董满祥,孙予罕,张启同.ReOxZrO2催化甲醇一步合成二甲氧基甲烷的研究[J].燃料化学学报,2007,35(3):334-338.
作者姓名:曹虎  郑岩  马珺  李军平  赵宁  王秀芝  魏伟  董满祥  孙予罕  张启同
作者单位:1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China; 2. Graduate School of the Chinese Academy of Sciences, Beijing , China; 3. Lanzhou Petroleum & Chemical Engineering Company, Lanzhou 730060, China;4. Feicheng Acid Chemicals Co. Ltd. Feicheng 271600, China
摘    要:利用负载型ReOxZrO2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。

关 键 词:二甲氧基甲烷  选择性氧化  铼氧化物  氧化锆  
文章编号:0253-2409(2007)03-0334-05
收稿时间:2006-11-06
修稿时间:2006年11月6日

One-step synthesis of dimethoxymethane from methanol over ReOx/ZrO2
CAO Hu,ZHENG Yan,MA Jun,LI Jun-ping,ZHAO Ning,WANG Xiu-zhi,WEI Wei,DONG Man-xiang,SUN Yu-han,ZHANG Qi-tong.One-step synthesis of dimethoxymethane from methanol over ReOx/ZrO2[J].Journal of Fuel Chemistry and Technology,2007,35(3):334-338.
Authors:CAO Hu  ZHENG Yan  MA Jun  LI Jun-ping  ZHAO Ning  WANG Xiu-zhi  WEI Wei  DONG Man-xiang  SUN Yu-han  ZHANG Qi-tong
Abstract: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.
Keywords:dimethoxymethane  selective oxidation  methanol  rhenium oxide  zirconia
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