物理化学学报 >> 2017, Vol. 33 >> Issue (8): 1699-1708.doi: 10.3866/PKU.WHXB201704263

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蒸氨法制备铜硅催化剂的二甲醚水蒸气重整制氢性能

王新雷1,马奎1,郭丽红1,2,丁彤1,程庆鹏1,田野1,*(),李新刚1,*()   

  1. 1 天津化学化工协同创新中心,天津市应用催化科学与工程重点实验室,天津大学化工学院,天津300354
    2 河南工业大学化学化工学院,郑州450001
  • 收稿日期:2017-03-13 发布日期:2017-06-14
  • 通讯作者: 田野,李新刚 E-mail:tianye@tju.edu.cn;xingang_li@tju.edu.cn
  • 基金资助:
    国家自然科学基金(21476159);国家自然科学基金(21476160);天津市自然科学基金(15JCZDJC37400);天津市自然科学基金(15JCYBJC23000)

Catalytic Performance for Hydrogen Production through Steam Reforming of Dimethyl Ether over Silica Supported Copper Catalysts Synthesized by Ammonia Evaporation Method

Xin-Lei WANG1,Kui MA1,Li-Hong GUO1,2,Tong DING1,Qing-Peng CHENG1,Ye TIAN1,*(),Xin-Gang LI1,*()   

  1. 1 Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300354, P. R. China
    2 School of Chemistry and Chemical Engineering, Henan University of Technology, Zhengzhou 450001, P. R. China
  • Received:2017-03-13 Published:2017-06-14
  • Contact: Ye TIAN,Xin-Gang LI E-mail:tianye@tju.edu.cn;xingang_li@tju.edu.cn
  • Supported by:
    The project was supported by the National Natural Science Foundation of China(21476159);The project was supported by the National Natural Science Foundation of China(21476160);Natural Science Foundation of Tianjin(15JCZDJC37400);Natural Science Foundation of Tianjin(15JCYBJC23000)

摘要:

采用蒸氨法制备出不同Cu负载量的xCu/SiO2-AE催化剂,并将其用于二甲醚水蒸气重整制氢反应。当Cu负载量为30%(w)时,30Cu/SiO2-AE催化剂表现出最佳的催化性能。结果显示,该方法制备的催化剂表面具有高度分散的Cu0和层状硅酸铜物相,经还原后分别形成Cu0和Cu+物种。与常规浸渍法制备的30Cu/SiO2-IM催化剂相比,蒸氨法制备的30Cu/SiO2-AE催化剂具有优异的催化稳定性和活性,这与其独特的层状结构和表面Cu0与Cu+之间的协同作用相关。

关键词: 二甲醚水蒸气重整, 制氢, 层状硅酸铜, Cu/SiO2, 蒸氨法

Abstract:

A series of xCu/SiO2-AE catalysts with different Cu loadings was prepared by the ammonia evaporation method. The as-prepared catalysts were used for hydrogen production via steam reforming of dimethyl ether, and showed high catalytic activities. The 30Cu/SiO2-AE catalyst (with 30% (w) Cu loading) exhibits the best catalytic performance. Our studies reveal the presence of highly dispersed Cu0 and copper phyllosilicate on the surface of the catalysts, which can then be reduced to Cu0 and Cu+ species, respectively. Compared with the 30Cu/SiO2-IM catalyst prepared by the conventional impregnation method, the remarkable catalytic stability and activity of the 30Cu/SiO2-AE catalyst are mainly ascribed to its unique lamellar structure and the cooperative effect between the surface Cu0 and Cu+ species.

Key words: Steam reforming of dimethyl ether, Hydrogen production, Copper phyllosilicate, Cu/SiO2, Ammonia evaporation method

MSC2000: 

  • O643