Cu-ZnO-ZrO2甲醇水蒸气重整催化剂的原位Raman表征

化学学报 ›› 2004, Vol. 62 ›› Issue (18): 1729-1732. 上一篇下一篇

研究论文

Cu-ZnO-ZrO₂甲醇水蒸气重整催化剂的原位Raman表征

云虹, 张慧, 陈建华, 陈鸿博

厦门大学化学系, 物理化学国家重点实验室, 厦门, 361005

投稿日期:2004-04-01 修回日期:2004-07-25 发布日期:2014-02-17
通讯作者: 陈鸿博,E-mail:hbchen@jingxian.xmu.edu.cn;Tel:013600934120 E-mail:hbchen@jingxian.xmu.edu.cn
基金资助:
福建省科学基金重大项目(No.2003H008)和厦门市科技计划项目(No.3502Z20021087)资助.

Characterization of Cu-ZnO-ZrO₂ Catalysts for Stream Reforming of Methanol by in situ Raman Spectroscopy

YUN Hong, ZHANG Hui, CHEN Jian-Hua, CHEN Hong-Bo

State Key Laboratory for Physical Chemistry of the Solid Surface, Department of Chemistry, Xiamen University, Xiamen 361005

Received:2004-04-01 Revised:2004-07-25 Published:2014-02-17

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摘要/Abstract

应用显微Raman光谱对Cu-ZnO-ZrO₂(Zr 24%,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544.8和652.8cm^-1分别为CuO-ZnO和ZrO₂的Raman吸收峰,而1361.8 cm^-1为HCOO-Cu对称伸缩振动吸收峰,在1590.3 cm^-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1350 cm^-1和分别在1550,1585,1595cm^-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.

关键词: Cu-ZnO-ZrO₂催化剂, 甲醇水蒸气重整, 甲醇合成, 显微Raman光谱

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.

Key words: Cu-ZnO-ZrO₂, stream reforming of methanol, methanol synthesis, in situ Raman spectroscopy

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云虹, 张慧, 陈建华, 陈鸿博. Cu-ZnO-ZrO₂甲醇水蒸气重整催化剂的原位Raman表征[J]. 化学学报, 2004, 62(18): 1729-1732.

YUN Hong, ZHANG Hui, CHEN Jian-Hua, CHEN Hong-Bo. Characterization of Cu-ZnO-ZrO₂ Catalysts for Stream Reforming of Methanol by in situ Raman Spectroscopy[J]. Acta Chimica Sinica, 2004, 62(18): 1729-1732.

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Cu-ZnO-ZrO₂甲醇水蒸气重整催化剂的原位Raman表征

Characterization of Cu-ZnO-ZrO₂ Catalysts for Stream Reforming of Methanol by in situ Raman Spectroscopy

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