物理化学学报 >> 2017, Vol. 33 >> Issue (6): 1123-1129.doi: 10.3866/PKU.WHXB201703301

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负载型双金属催化剂的制备及其等离子体催化氨分解制氢性能

孙帅其1,易颜辉1,王丽1,张家良2,郭洪臣1,*()   

  1. 1 大连理工大学化工学院催化化学与工程系,精细化工国家重点实验室,辽宁大连116024
    2 大连理工大学物理与光电工程学院,辽宁大连116024
  • 收稿日期:2017-02-28 发布日期:2017-05-19
  • 通讯作者: 郭洪臣 E-mail:hongchenguo@163.com
  • 基金资助:
    国家自然科学基金(20473016);国家自然科学基金(20673018)

Preparation and Performance of Supported Bimetallic Catalysts for Hydrogen Production from Ammonia Decomposition by Plasma Catalysis

Shuai-Qi SUN1,Yan-Hui YI1,Li WANG1,Jia-Liang ZHANG2,Hong-Chen GUO1,*()   

  1. 1 State Key Laboratory of Fine Chemicals, Department of Catalytic Chemistry and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China
    2 School of Physics and Optoelectronic Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China
  • Received:2017-02-28 Published:2017-05-19
  • Contact: Hong-Chen GUO E-mail:hongchenguo@163.com
  • Supported by:
    The project was supported by the National Natural Science Foundation of China(20473016);The project was supported by the National Natural Science Foundation of China(20673018)

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摘要：

利用等体积浸渍法制备了Fe-Co、Fe-Ni、Mo-Co、Mo-Ni双金属催化剂(总金属含量均为10%(w，质量分数)，双金属摩尔比均为1:1)，考察了其在等离子体条件下氨分解活性，结果表明Fe-Ni双金属催化剂表现出较好的协同作用。在此基础上，进一步考察了Fe/Ni摩尔比对其活性的影响。结果表明：当Fe/Ni摩尔比为6/4时，氨分解活性最好，而且该双金属催化剂稳定性良好。采用N2物理吸附、X射线衍射(XRD)、H2-程序升温还原(H2-TPR)和高分辨透射电子显微镜(HRTEM)对催化剂的物化性质、还原性能、微观形貌等进行了研究。结果表明：活性较好的Fe-Ni双金属催化剂中，Fe与Ni形成尖晶石结构NiFe2O4，该结构有利于Fe和Ni的还原，即活性组分易恢复金属态，这可能是其活性较高的原因。

关键词: 等离子体, Fe-Ni, 双金属催化剂, 氨分解, 氢气

Abstract:

Bimetallic Fe-Co, Fe-Ni, Mo-Co, and Mo-Ni catalysts, with total metal contents of 10 wt% and bimetallic molar ratios of 1:1, were prepared by the incipient wetness impregnation method and their activities for ammonia decomposition in the presence of plasma were studied. The Fe-Ni bimetallic catalyst exhibited a better synergistic effect than the other three bimetallic catalysts. The effect of the Fe/Ni molar ratio on its catalytic activity was also investigated. A 6:4 Fe/Ni molar ratio resulted in the highest ammonia decomposition activity and stability. The catalysts were characterized by N2 adsorption-desorption, XRD, H2-TPR, and HRTEM. The characterization results indicated that NiFe2O4 with a spinel structure was formed in the optimal Fe-Ni bimetallic catalysts and this structure favors the reduction of Fe and Ni. In other words, it is easy to achieve the metallic state of active components for the Fe-Ni bimetallic catalysts, which could be the reason for the high catalytic activity of bimetallic catalysts for NH3 decomposition.

Key words: Plasma, Fe-Ni, Bimetallic catalysts, Ammonia decomposition, Hydrogen