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EDTA修飾對(duì)Ru/Ba-MgO氨合成催化劑性能的影響及作用機(jī)理
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浙江工業(yè)大學(xué)化學(xué)工程學(xué)院,浙江工業(yè)大學(xué)化學(xué)工程學(xué)院,浙江工業(yè)大學(xué)化學(xué)工程學(xué)院

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浙江省公益性技術(shù)應(yīng)用研究(分析測(cè)試)計(jì)劃項(xiàng)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:

    利用超聲——共沉淀技術(shù)制備了一系列EDTA修飾的摻鋇納米氧化鎂載體(EDTA-Ba-MgO)及其負(fù)載的釕基氨合成催化劑(Ru/EDTA-Ba-MgO)。通過場(chǎng)發(fā)射掃描電鏡、X射線粉末衍射、氮物理吸附、熱重分析儀及H2程序升溫還原等方法對(duì)載體/催化劑進(jìn)行表征,結(jié)果表明:EDTA的修飾作用改變了鋇助劑與載體的作用方式,通過與Ba助劑發(fā)生絡(luò)合作用形成了[Ba(EDTA)]2-,改變了Ba2 的帶電性質(zhì),使鋇助劑在帶正電荷的載體表面實(shí)現(xiàn)了直接吸附,從而更有利于對(duì)鋇助劑在Ba-MgO中摻雜量及摻雜形式的調(diào)控,最終達(dá)到提高催化劑活性的目的。在10 MPa,10000 h?1和425 篊的反應(yīng)條件下,Ru/EDTA-Ba-MgO催化劑上氨合成速率達(dá)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,程向煒,杜彥磊. EDTA修飾對(duì)Ru/Ba-MgO氨合成催化劑性能的影響及作用機(jī)理[J].稀有金屬材料與工程,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
  • 錄用日期:2015-01-13
  • 在線發(fā)布日期: 2017-05-18
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