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Platinum supported on [60]fullerene-grafted silica as a new potential catalyst for hydrogenation

机译:铂负载在[60]富勒烯接枝的二氧化硅上作为氢化的新潜在催化剂

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A Pt-based catalyst supported on a silica grafted with [60]fullerene was prepared and evaluated in the liquid-phase hydrogenation of cinnamaldehyde. Silanization of a large-pore silica was carried out with diethoxymethylsilane. [60]Fullerene was anchored on the modified silica through a hydrosilylation reaction with Si-H bonds, mediated by a Pt-0 Karsted catalyst. IR, Si-29 and C-13 MAS NMR spectroscopies, and N-2 adsorption-desorption provided evidence that [60]fullerene was covalently bonded onto the silica surface. [60]Fullerene was released at ca 950, 750, and 800 K in He, air, and H-2, respectively, even in the presence of 0.8 wt% Pt. The very high density of [60]fullerene grafting confers a strong hydrophobic character to the surface. A fairly good selectivity to cinnamyl alcohol was observed on this catalyst at cinnamaldehyde conversion above 90%. This behavior might be better explained by a specific interaction between the phenyl ring of cinnamaldehyde and the grafted [60]fullerene film than by a modification of the Pt d-band. The IR spectroscopy of adsorbed CO did not provide any evidence of an enhanced, or reduced, back-donation to 2 pi* antibonding orbitals of CO, with respect to classical supported Pt catalysts. (C) 1998 Academic Press. [References: 20]
机译:制备了负载在接枝有[60]富勒烯的二氧化硅上的Pt基催化剂,并在肉桂醛的液相加氢中进行了评估。用二乙氧基甲基硅烷对大孔二氧化硅进行硅烷化。 [60]富勒烯通过具有Pt-0 Karsted催化剂介导的具有Si-H键的氢化硅烷化反应而固定在改性的二氧化硅上。 IR,Si-29和C-13 MAS NMR谱图以及N-2吸附-解吸提供了[60]富勒烯共价键合到二氧化硅表面的证据。 [60]即使存在0.8 wt%的Pt,富勒烯也分别在大约950、750和800 K的He,空气和H-2中释放。 [60]富勒烯接枝的极高密度赋予其表面很强的疏水性。在肉桂醛转化率高于90%时,在该催化剂上观察到对肉桂醇的相当好的选择性。这种行为可能是通过肉桂醛的苯环与接枝的[60]富勒烯薄膜之间的特定相互作用比通过修饰Pt d波段更好地解释的。相对于传统的负载型Pt催化剂,吸附的CO的IR光谱未提供任何证据表明将CO的反向捐赠增加或减少至2 pi *反键轨道。 (C)1998年学术出版社。 [参考:20]

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