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Selective 1,3-butadiene hydrogenation by gold nanoparticles deposited & precipitated onto nanocarbon materials

机译:通过沉积的金纳米粒子选择1,3-丁二烯氢化并沉淀到纳米碳材料上

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摘要

Graphene oxide and multiwall carbon nanotubes (CNTs) were chemically modified by treatment with urea and subsequent annealing at different temperatures. These materials were used as supports for gold nanoparticles and the resulting samples have been applied as catalysts in the 1,3-butadiene partial hydrogenation reaction. The supports and catalysts were exhaustively characterized. It was shown that urea treatments modified the graphene surfaces and the morphology of CNTs, in both cases with incorporation of significant amounts of different nitrogen surface groups. The presence of these groups on few layered graphene or on CNT surfaces modifies the gold precipitation-deposition process during catalyst preparation, giving place to different amounts of incorporated gold on the various supports. The obtained catalytic results suggested that the partial hydrogenation requires limited availability of hydrogen, and for this the migration through adsorbed species between the metal and support to initiate the hydrogenation, probably by a spillover mechanism, seems to be a required step. In general intramolecular selectivity is structure-sensitive meanwhile catalytic activity is not structure-sensitive, as evidenced when the gold nanoparticle sizes are decreased.
机译:通过用尿素处理和随后在不同温度下的退火进行化学改性石墨烯氧化物和多壁碳纳米管(CNT)。这些材料被用作金纳米颗粒的载体,并将所得样品在1,3-丁二烯部分氢化反应中施加为催化剂。备注和催化剂被详尽地表征。结果表明,在两种情况下,尿素处理改性了石墨烯表面和CNT的形态,其掺入大量不同的氮表面基团。在少数层状石墨烯或CNT表面上存在这些基团的存在改变催化剂制剂期间的金沉淀沉积过程,在各种载体上给出不同量的掺入金。所获得的催化结果表明,部分氢化需要有限的氢的可用性,并且对于金属和载体之间的吸附物质的迁移,以引发氢化,可能是通过溢出机制,似乎是所需的步骤。在一般的分子内选择性是结构敏感的同时催化活性不是结构敏感的,如在金纳米颗粒尺寸下降时所证明的。

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  • 来源
    《RSC Advances》 |2015年第99期|共16页
  • 作者单位

    UNED Fac Ciencias Dept Quim Inorgan &

    Quim Tecn Madrid 28040 Spain;

    Unidad Asociada UNED CSIC Grp Design &

    Applicat Heterogeneous Catalysts Madrid Spain;

    UNED Fac Ciencias Dept Quim Inorgan &

    Quim Tecn Madrid 28040 Spain;

    UNED Fac Ciencias Dept Quim Inorgan &

    Quim Tecn Madrid 28040 Spain;

    Unidad Asociada UNED CSIC Grp Design &

    Applicat Heterogeneous Catalysts Madrid Spain;

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

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