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Ethanol dehydrogenative reactions catalyzed by copper supported on porous Al-Mg mixed oxides

机译:通过铜催化的乙醇脱氢反应在多孔Al-Mg混合氧化物上催化

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摘要

Mixed aluminum and magnesium oxides (AlMgO) prepared by means of an emulsion-mediated sol-gel method was impregnated with copper nitrate solution and used in the ethanol dehydrogenative reactions to produce acetaldehyde and ethyl acetate. The emulsified system allowed to obtain a macro-mesoporous support that resulted in an outstanding dispersion of copper. The porous catalyst was about 3 times more active than the non-porous counterpart, due to the formation on the support's surface of Cu-0 together with the more active Cu+ species. In fact, the simultaneous presence of Cu+ and Cu-0 were advantageous for the catalytic performance, as the turnover frequencies, were 122 and 166 h(-1) for the non-porous reference catalyst and for the porous one, respectively. Both catalysts deactivated due to copper particles sintering, however the porous one deactivated less, as a consequence of the better dispersion of the Cu species on the macro and mesoporous support. Acetaldehyde was the main product, however by increasing the contact time by 6.6 times, the conversion of ethanol on the nonporous catalyst reached about 90% with a selectivity to ethyl acetate of 20% by means of the coupling reaction of ethanol and acetaldehyde. The selectivity to ethyl acetate was favoured on an increased support/copper interface that is given by larger copper particles.
机译:通过乳液介导的溶胶方法制备的混合铝和氧化镁(ALMGO)用硝酸铜溶液浸渍并用于乙醇脱氢反应,得到乙醛和乙酸乙酯。乳化系统使得获得宏观介孔的载体,导致铜的出色分散。由于Cu-0的表面上与更活性的Cu +物种一起形成,多孔催化剂比无孔对应物更活跃的约3倍。实际上,Cu +和Cu-0的同时存在对于非多孔参考催化剂的转换频率为122和166h(-1),以及多孔一体的催化性能分别是有利的。由于铜颗粒烧结,两种催化剂都是失活的,然而,多孔单次失活,因为Cu物种在宏观和中孔载体上更好地分散。乙醛是主要产物,然而,通过将接触时间提高6.6倍,乙醇对无孔催化剂的转化率达到约90%,通过乙醇和乙醛的偶联反应选择性为20%的乙酸乙酯。对乙酸乙酯的选择性有利于由较大的铜颗粒给出的载体/铜界面增加。

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  • 来源
    《RSC Advances》 |2019年第6期|共9页
  • 作者单位

    Univ Estadual Paulista UNESP Inst Quim R Prof Francisco Degni 55 BR-14800900 Araraquara SP Brazil;

    Inst Fed Sao Paulo Campus Avare Av Prof Celso Ferreira da Silva 1333 BR-18707150 Avare SP Brazil;

    Univ Fed Sao Carlos Ctr Pesquisas Mat Avancados &

    Energia Rodovia Washington Luis Km 235 BR-13565905 Sao Carlos SP Brazil;

    Univ Fed Sao Carlos Ctr Pesquisas Mat Avancados &

    Energia Rodovia Washington Luis Km 235 BR-13565905 Sao Carlos SP Brazil;

    Univ Estadual Paulista UNESP Inst Quim R Prof Francisco Degni 55 BR-14800900 Araraquara SP Brazil;

    Univ Estadual Paulista UNESP Inst Quim R Prof Francisco Degni 55 BR-14800900 Araraquara SP Brazil;

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