CaO改性对CuZnAlZr催化剂在合成气制低碳醇中性能的影响

doi:10.3866/PKU.WHXB201203302

物理化学学报 >> 2012, Vol. 28 >> Issue (06): 1461-1466.doi: 10.3866/PKU.WHXB201203302

CaO改性对CuZnAlZr催化剂在合成气制低碳醇中性能的影响

朱秋锋, 张荣俊, 贺德华

清华大学化学系, 有机光电子与分子工程教育部重点实验室, 分子催化与定向转化研究室, 北京 100084

收稿日期:2012-01-07 修回日期:2012-03-14 发布日期:2012-05-17
通讯作者: 贺德华 E-mail:hedeh@mail.tsinghua.edu.cn
基金资助:
国家高技术研究发展计划(863)(2007AA05Z332)资助项目

Effect of CaO Modification on Performance of CuZnAlZr Catalyst in Synthesis of Higher Alcohols from Synthesis Gas

ZHU Qiu-Feng, ZHANG Rong-Jun, HE De-Hua

Innovative Catalysis Program, Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China

Received:2012-01-07 Revised:2012-03-14 Published:2012-05-17
Contact: HE De-Hua E-mail:hedeh@mail.tsinghua.edu.cn
Supported by:
The project was supported by the National High Technology Research and Development Program of China (863) (2007AA05Z332).

摘要/Abstract

摘要： 采用机械混合法和共沉淀法制备了CaO改性CuZnAlZr 氧化物催化剂, 在高压微型固定床反应器上考察了其在合成气制低碳醇反应中的催化性能, 利用粉末X射线衍射(XRD)、低温氮气吸附-脱附、H₂程序升温还原(H₂-TPR)和二氧化碳吸附-脱附(CO₂-TPD)等技术对催化剂进行了表征. 结果显示: CaO改性对CuZnAlZr 催化剂的织构性质没有明显的影响; 但共沉淀法制备的CaO改性CuZnAlZr 催化剂具有弱碱性和中等强度两种碱性中心, 且有较多的碱中心数量; 而未改性的CuZnAlZr 催化剂只具有弱碱性中心. CO加氢反应结果表明:经共沉淀法制备的CaO改性CuZnAlZr催化剂对C₂₊醇的生成有明显的促进作用.

关键词: CaO改性, CuZnAlZr催化剂, 合成气, 低碳醇

Abstract: CaO modified CuZnAlZr mixed oxide catalysts were prepared by mechanical mixing and co-precipitation methods, and their catalytic performances for CO hydrogenation to higher alcohols were investigated using a continuous flow high-pressure fixed-bed micro-reactor. The catalysts were characterized by X-ray diffraction (XRD), N₂-adsorption-desorpotion, temperature-programmed reduction of H₂ (H₂-TPR), and temperature-programmed desorption of CO₂ (CO₂-TPD). The results showed that doping with CaO did not alter the textural properties of the catalyst, but increased the number of basic sites. Furthermore, the CaO-modified CuZnAlZr catalysts possessed both weak and medium strength basic sites, while unmodified CuZnAlZr catalyst possessed only weak basic sites. Catalytic performance, assessed by CO hydrogenation to C₂₊ alcohols, was improved in the CaO-doped CuZnAlZr catalyst relative to the undoped catalyst.

Key words: CaO modification, CuZnAlZr catalyst, Synthesis gas, Higher alcohol

朱秋锋, 张荣俊, 贺德华. CaO改性对CuZnAlZr催化剂在合成气制低碳醇中性能的影响[J]. 物理化学学报, 2012, 28(06), 1461-1466. doi: 10.3866/PKU.WHXB201203302

ZHU Qiu-Feng, ZHANG Rong-Jun, HE De-Hua. Effect of CaO Modification on Performance of CuZnAlZr Catalyst in Synthesis of Higher Alcohols from Synthesis Gas[J]. Acta Phys. -Chim. Sin. 2012, 28(06), 1461-1466. doi: 10.3866/PKU.WHXB201203302

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201203302

https://www.whxb.pku.edu.cn/CN/Y2012/V28/I06/1461

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CaO改性对CuZnAlZr催化剂在合成气制低碳醇中性能的影响

Effect of CaO Modification on Performance of CuZnAlZr Catalyst in Synthesis of Higher Alcohols from Synthesis Gas

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