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作 者:杨意泉[1] 方雪明[1] 李晨[1] 程大典[1] 袁友珠[1] 林仁存[1] 张鸿斌[1]
机构地区:[1]厦门大学化学系
出 处:《厦门大学学报(自然科学版)》2001年第6期1251-1255,共5页Journal of Xiamen University:Natural Science
基 金:厦门大学固体表面物理化学国家重点实验室资助项目 (990 7)
摘 要:在 Cu- Zn- Al甲醇合成催化剂中添加适量的氧化锆助剂 ,制得 Cu- Zn- Al- Zr催化剂及表征其特性 .实验结果表明 ,Cu- Zn- Al- Zr催化剂最佳反应温度为 2 30℃ ,比 Cu- Zn- Al低约 10℃ ;热处理前后甲醇得率分别比 Cu- Zn- Al高 16%和 38% .UVDR表征显示 ,反应后催化剂在 5 98nm处观测到在 Zn O晶格介面上的 Cu+;CO- TPD表征显示 ,经 4 5 0℃热处理后的催化剂只在 182℃~ 197℃处出现一个由 Cu0 位贡献的吸附峰 ,热处理前在 2 61℃~ 2 74℃处由 Cu+位贡献的吸附峰消失 .Cu-Zn- Al- Zr催化剂对 CO的吸附量和 Cu+含量均大于 Cu- Zn- Al催化剂 。The principle of ion doping and valence compensation was adopted to develop a new catalyst Cu-Zn-Al-Zr which was derived from traditional Cu-Zn-Al catalyst by adding a small amount of ZrO_2 for MeOH synthesis under low pressure. The catalytic properties of the catalyst for the reaction were measured. The results show that the optimum reaction temperature is found to be 230 ℃, lower by 10 ℃ than that on the Cu-Zn-Al catalyst. On the catalysts without undergoing a heat-treatment, the yield of MeOH is higher by 16% than that on the Cu-Zn-Al catalyst. However, on the catalysts undergoing a heat-treatment, the yield is higher by 38%. It can be seen from the UV-Visible spectra that the Cu^+ species on the surface of ZnO as a band appeared at 598 nm in functioning state of the catalysts. The CO-TPD shows that there is only an absorbed peak which can be attributed to Cu^0, at temperature of 182 ℃~197 ℃ after the catalysts were calcined at 450 ℃, meanwhile the absorbed peak attributed to Cu^+ at 261 ℃~274 ℃ disappeared. The adsorbed volume of CO and the amount of Cu^+ for Cu-Zn-Al-Zr are all found to be higher than for Cu-Zn-Al catalyst. This probably is reasons for their higher activity at low temperature and the better thermostablity for the catalyst Cu-Zn-Al-Zr.
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