Cu-ZnO-ZrO_2甲醇水蒸气重整催化剂的原位Raman表征  

Characterization of Cu-ZnO-ZrO_2 Catalysts for Stream Reforming of Methanol by in situ Raman Spectroscopy

作　　者：云虹[1] 张慧[1] 陈建华[1] 陈鸿博[1] 

机构地区：[1]厦门大学化学系物理化学国家重点实验室,厦门361005

出　　处：《化学学报》2004年第18期1729-1732,共4页Acta Chimica Sinica

基　　金：福建省科学基金重大项目 (No .2 0 0 3H0 0 8);厦门市科技计划项目 (No .350 2Z2 0 0 2 1 0 87)资助

摘　　要：应用显微Raman光谱对Cu ZnO ZrO2 (Zr 2 4% ,w)催化剂催化甲醇水蒸气重整 (SRM)反应进行原位表征 ,并将结果与相同催化剂上的甲醇合成 (MS)反应进行对比 ,结果表明 :在SRM反应时 ,催化剂表面出现四个宽峰 ,其中 5 44 8和 65 2 8cm-1分别为CuO ZnO和ZrO2 的Raman吸收峰 ,而 13 61 8cm-1为HCOO—Cu对称伸缩振动吸收峰 ,在 15 90 3cm-1附近的谱峰归属于甲酸物种中OCO的不对称伸缩振动 .在由CO CO2 H2 合成气合成甲醇时 ,在 13 5 0cm-1和分别在 15 5 0 ,15 85 ,15 95cm-1出现两个甲酸根表面物种和甲酸盐的振动吸收谱带 .因此 ,在Cu ZnO ZrO2 催化剂上的甲醇合成和甲醇水蒸气重整存在相同的甲酸根中间体 ,这一结果将有助于对甲醇合成和甲醇水蒸气重整反应机理的理解 .Characterization of Cu-ZnO-ZrO2 catalysts for stream reforming of methanol (SRM) by in situ Raman spectroscopy has been done. The results have been contrasted with those from reaction of methanol synthesis (MS) over the same catalysts. The results indicated that there are four Raman peaks on the surface of the catalyst for SRM reaction. The Raman spectra of 544.8 cm(-1) were assigned to CuO-ZnO, 652.8 cm(-1) to ZrO2, 1361.8 cm(-1) to symmetry flex oscillatory adsorption of HCOO-Cu and 1590.3 cm(-1) to asymmetry flex oscillatory adsorption of OCO in formic acid species, respectively. The peak of 1350 cm(-1) and three peaks of 1550, 1585 and 1595 cm(-1) were assigned to Raman flex adsorbed band of formic acidic group and formic acidic salt on surface of catalyst for methanol synthesis. So formic acidic group existed on the surface of the catalysts for SRM and MS reactions. This result has an important significance for mechanism knowledge of SRM and MS reactions.

关 键 词：甲醇 水蒸气重整 显微Raman光谱 铜-氧化锌-氧化铬催化剂 合成 

分 类 号：O643.3[理学—物理化学]