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Effects of metal promotion on CuMgFe catalysts derived from layered double hydroxides for higher alcohol synthesis via syngas

机译:金属促进对衍生自分层双氢氧化物衍生的Cumgfe催化剂的影响通过合成气升高醇合成

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摘要

Cu-Mg-Fe-M-O (M = Mn, Zr, and Ce) catalysts derived from layered double hydroxides (LDHs) precursors were prepared using a co-precipitation method and tested for higher alcohol synthesis (HAS) via carbon monoxide hydrogenation. The catalysts were subsequently characterized by N-2-physisorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and H-2 temperature-programed reduction (H-2-TPR). The results show that Mn, Zr, and Ce promoters mainly contribute to the formation of tetrahedrally coordinated copper species, which favor the enhancement of the total alcohol selectivity. The addition of Mn facilitates the interaction between Cu and Fe, which causes the total alcohol selectivity and C2+ alcohol content in the total alcohols increased from 9.82% and 68.85% to 15.1% and 73.14%, respectively. However, the addition of Zr and Ce weakens the Cu-Fe interaction but increases the possibility of contact between Cu and Fe. As a consequence, the total alcohol selectivity is enhanced, while the C2+ alcohol content in the total alcohols is reduced upon Zr and Ce addition. Based on the characterization and catalytic results of the catalysts, a triple-active-site model is proposed to explain the different promoting effects of the three additives.
机译:使用共沉淀法制制备从层状双氢氧化物(LDHS)前体的Cu-Mg-Fe-M-O(m = Mn,Zr和Ce)催化剂,并通过一氧化碳氢化测试以获得更高的醇合成(具有)。随后将催化剂的特征在于N-2 - 物理吸附,X射线衍射(XRD),透射电子显微镜(TEM),X射线光电子能谱(XPS)和H-2温度编程减少(H-2-TPR) 。结果表明,Mn,Zr和Ce启动子主要有助于形成四面体协调的铜物质,这有利于增强全部酒精选择性。添加Mn促进Cu和Fe之间的相互作用,这导致总醇的总醇选择性和总醇中的C2 +醇含量分别从9.82%增加到15.1%和73.14%。然而,添加Zr和Ce削弱了Cu-Fe相互作用,但增加了Cu和Fe之间接触的可能性。结果,增强了总醇选择性,而总醇中的C2 +醇含量降低,并加入总醇。基于催化剂的表征和催化结果,提出了一种三效位的模型来解释三种添加剂的不同促进作用。

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  • 来源
    《RSC Advances》 |2015年第64期|共7页
  • 作者单位

    Chinese Acad Sci Inst Coal Chem State Key Lab Coal Convers Taiyuan 030001 Shanxi Peoples R China;

    Chinese Acad Sci Inst Coal Chem State Key Lab Coal Convers Taiyuan 030001 Shanxi Peoples R China;

    Chinese Acad Sci Inst Coal Chem State Key Lab Coal Convers Taiyuan 030001 Shanxi Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
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