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EDTA修饰对Ru/Ba-MgO氨合成催化剂性能的影响及作用机理
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浙江工业大学化学工程学院,浙江工业大学化学工程学院,浙江工业大学化学工程学院

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浙江省公益性技术应用研究(分析测试)计划项目(2014C37048)


Influence of Ethylene Diamine Tetraacetic Acid on the Performance of Magnesia Supported Ru-based Catalysts for Ammonia Synthe
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College of Chemical Engineering, Zhejiang University of Technology,College of Chemical Engineering, Zhejiang University of Technology,College of Chemical Engineering, Zhejiang University of Technology

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Supported by the public technology research(Test) program of Zhejiang Province, China (2014C37048)

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    摘要:

    利用超声——共沉淀技术制备了一系列EDTA修饰的掺钡纳米氧化镁载体(EDTA-Ba-MgO)及其负载的钌基氨合成催化剂(Ru/EDTA-Ba-MgO)。通过场发射扫描电镜、X射线粉末衍射、氮物理吸附、热重分析仪及H2程序升温还原等方法对载体/催化剂进行表征,结果表明:EDTA的修饰作用改变了钡助剂与载体的作用方式,通过与Ba助剂发生络合作用形成了[Ba(EDTA)]2-,改变了Ba2 的带电性质,使钡助剂在带正电荷的载体表面实现了直接吸附,从而更有利于对钡助剂在Ba-MgO中掺杂量及掺杂形式的调控,最终达到提高催化剂活性的目的。在10 MPa,10000 h?1和425 篊的反应条件下,Ru/EDTA-Ba-MgO催化剂上氨合成速率达到 60.27 mmol/(g?h),比Ru/Ba-MgO提高了7.4%。

    Abstract:

    A series of barium doped nano-magnesia supports (Ba-MgO) modified with EDTA were prepared by chemical co-precipitation with ultrasonic method and were used as supports to prepare Ru-based catalysts. The surface texture and the matter phase of the supports and Ru catalysts were characterized by X-ray diffraction, scanning electron microscope, N2 physical-adsorption, H2 temperature-programmed reduction and inductively coupled plasma-atomic emission spectrometry respectively. The results showed that modification of EDTA increased the amount of barium promoter into the support and controlled the formation state of barium in support. The effects of barium promoter content and surface texture in support achieved an equilibrium state when the molar ratio of EDTA to Ba was 1/2, and the highest activity of Ru/Ba-MgO catalyst was 69.31 mmol g-1h-1 under the reaction conditions of 10 MPa, 10 000 h-1 and 698 K.

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霍超,程向炜,杜彦磊. EDTA修饰对Ru/Ba-MgO氨合成催化剂性能的影响及作用机理[J].稀有金属材料与工程,2017,46(3):657~662.[Huo Chao, Cheng Xiangwei, Du Yanlei. Influence of Ethylene Diamine Tetraacetic Acid on the Performance of Magnesia Supported Ru-based Catalysts for Ammonia Synthe[J]. Rare Metal Materials and Engineering,2017,46(3):657~662.]
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  • 收稿日期:2014-11-27
  • 最后修改日期:2014-12-28
  • 录用日期:2015-01-13
  • 在线发布日期: 2017-05-18
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