ZrO2在Cu-ZnO-ZrO2甲醇水蒸汽重整制氢催化剂中的作用

通过对一系列Cu-ZnO-ZrO2甲醇水蒸汽重整(SRM)催化剂的XRD、TEM和BET表征及催化性能测定,研究催化剂中ZrO2对催化剂粒径、比表面以及对SRM反应性能的影响.结果表明,ZrO2的加入,使催化剂的粒径从15 nm降至10 nm（其中CuO和ZnO的平均粒径分别从7.7和10.4 nm降至3.9和8.7 nm）,BET比表面从60 m2•g－1增至78 m2•g－1.随着催化剂含ZrO2量不同,甲醇的转化率和H2、CO2的选择性均产生变化,当催化剂中Zr含量为24.0％(w),反应温度为220 ℃,水、醇摩尔比为1.3时,甲醇的转化率达到51.6％, H2和CO2的选择性达到100％(CO和CH4在产物气体中的体积分数小于10－4),这一结果对甲醇燃料电池甲醇重整器的应用具有重要的意义.

The Effects of ZrO2 on Cu-ZnO-ZrO2 Catalysts for Hydrogen Generation by Steam Reforming of Methanol

The effects of Zr in CuO-ZnO-ZrO2 catalysts on the diameter of CuO and ZnO ,BET surface area of the catalysts as well as the catalytic activity have been studied by XRD,TEM,BET and the evaluation of catalytic activity for steam reforming of methanol (SRM).The results indicated that the diameter of catalyst particle was lowered from 15 to 10 nm (the average diameters of CuO and ZnO were lowered from 7.7 and 10.4 nm to 3.9 and 8.7 nm, respectively),the BET surface area was increased from 60 to 78 m2•g－1 due to the existence of Zr. The conversion of methanol and the sensitivity of both hydrogen and carbon dioxide over Cu-ZnO-ZrO2 catalysts in SRM reaction were changed along with content of Zr in the catalysts. The conversion of methanol of 51.6％ and the sensitivity of both hydrogen and carbon dioxide of 100％ (content of CO and CH4 was lower than 10－4(φ)and can not be detected by 102GC) were obtained under the following reaction conditions: Zr content of 24.0％(w) in the catalyst, reaction temperature of 220 ℃ and mole ratio of water to methanol of 1.3. These results have important significance in the application of steam reformer of methanol for methanol fuel cell.