物理化学学报 >> 2017, Vol. 33 >> Issue (9): 1865-1874.doi: 10.3866/PKU.WHXB201704285

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碳纤维负载Rh-Mn紧密接触的催化剂及其合成气制乙醇催化性能

宁红岩1,2,杨其磊1,2,杨晓1,2,李鹰霞1,2,宋兆钰1,2,鲁逸人3,张立红1,2,*(),刘源1,2,*()   

  1. 1 天津大学,天津市应用催化科学与工程重点实验室,天津300072
    2 化学工程与技术(天津)协同创新中心,天津300072
    3 天津大学环境科学与工程学院,天津300072
  • 收稿日期:2017-03-23 发布日期:2017-07-05
  • 通讯作者: 张立红,刘源 E-mail:zlh_224@tju.edu.cn;yuanliu@tju.edu.cn
  • 基金资助:
    化学资源有效利用国家重点实验室基金和国家自然科学基金(21576192);化学资源有效利用国家重点实验室基金和国家自然科学基金(21576192)

Carbon Fiber-supported Rh-Mn in Close Contact with Each Other and Its Catalytic Performance for Ethanol Synthesis from Syngas

Hong-Yan NING1,2,Qi-Lei YANG1,2,Xiao YANG1,2,Ying-Xia LI1,2,Zhao-Yu SONG1,2,Yi-Ren LU3,Li-Hong ZHANG1,2,*(),Yuan LIU1,2,*()   

  1. 1 Tianjin Key Laboratory for Applied Catalysis Science & Technology, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China
    2 Collaborative Innovation Center of Chemical Science & Engineering(Tianjin), Tianjin 300072, P. R. China
    3 School of Environmental Science and Engineering, Tianjin University, Tianjin 300072, P. R. China
  • Received:2017-03-23 Published:2017-07-05
  • Contact: Li-Hong ZHANG,Yuan LIU E-mail:zlh_224@tju.edu.cn;yuanliu@tju.edu.cn
  • Supported by:
    The project was supported by State Key Laboratory of Chemical Resource Engineering and National Natural Science Foundation of China(21576192);The project was supported by State Key Laboratory of Chemical Resource Engineering and National Natural Science Foundation of China(21576192)

摘要:

Rh-Mn基催化剂用于合成气制乙醇反应颇具潜力。本文采用柠檬酸乙二醇原位聚合的方法在碳纤维(CF)表面负载Rh-Mn催化剂。采用TPR,XRD,TEM,EDS,CO-TPD,H2脉冲吸附和XPS技术对焙烧和还原后样品的结构和物化性能进行了表征,并考察了催化剂催化合成气制乙醇的反应性能。结果表明,原位聚合法相比传统浸渍法更利于形成紧密接触的Rh-Mn物种,可有效提高Rh的分散度和抗烧结性,显著改善合成气转化反应中CO加氢活性和乙醇选择性。

关键词: Rh-Mn相互作用, 合成气, 乙醇合成, 碳纤维, CO加氢

Abstract:

Rh-Mn-based catalysts are promising for ethanol synthesis from syngas. In this work, a carbon fiber (CF)-supported Rh-Mn catalyst, with highly dispersed Rh and close contact Rh-Mn species, has been prepared by a new in situ polymerization route using citric acid and ethylene glycol interaction. The structure and physicochemical properties of both the calcined and reduced samples have been characterized by TPR, XRD, TEM, EDS, CO-TPD, H2 chemisorption, and XPS techniques and the catalytic performance for ethanol synthesis from syngas has been evaluated. The results show that the new method is beneficial in forming close contact Rh-Mn species than that obtained with the conventional impregnation method. This can enhance the dispersion and sintering resistance of Rh and effectively improve the activity of CO hydrogenation and the selectivity to ethanol in ethanol synthesis from syngas.

Key words: Close contact Rh-Mn, Syngas, Ethanol synthesis, Carbon fiber, CO hydrogenation

MSC2000: 

  • O643