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Au-Ni双金属纳米颗粒的固相可控合成及其在气相醇氧化中的应用
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摘要
本文报道了一种固相晶种的方法(通过在三维介孔SiO_2的孔道中先沉积镍盐和金纳米颗粒(AuNPs),再高温H_2/Ar还原。)来合成Au-Ni双金属纳米颗粒(BMNPs)。在该过程中,预负载的AuNPs作为镍盐还原生长的晶核,并且在高温条件下,二者进一步合金化,得到了尺寸均一的Au-Ni BMNPs。在Au-Ni金属相图的指导下,通过调节Au-Ni的投入比或者还原温度,可以得到不同组成和结构的Au-Ni BMNPs。并且,通过控制AuNPs的大小,Au-Ni BMNPs的尺寸也可以得到调控。动力学测试表明,Ni的引入能够提升Au对于氧气分子的活化能力,使得Au对于苯甲醇的气相氧化反应活性提高了5-6倍。
We report a general seed-mediated solid-state alloying strategy for Au-Ni BMNPs by depositing Nickel salts and AuN Ps into the EP-FDU-12 support before high-temperature reduction. Pre-loaded monodispersed MNPs played a role of seeds for the second metal growth, and alloyed with it under high temperature within well-defined 3-D mesostructures of the mesoporous supports. As a result, BMNPs of uniform size with narrow distribution were obtained. Besides, the structure of as prepared BMNPs could be designed under the direction of phase diagram, with their composition and size can be tuned as well. The Au-Ni BMNPs showed up-to 6-folds enhanced catalytic activity in gas phase alcohol oxidation.
引文
[1]B.D.Chandler,C.G.Long,J.D.Gilbertson,and K.J.Stevenson,J.Phy.Chem.C,2010,114:11498-11508.
    [2]C.C.Leon,J.-G.Lee and S.T.Ceyer,J.Phy.Chem.C,2014,118:29043-29057.

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