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首页> 外文期刊>RSC Advances >A magnetically recyclable superparamagnetic silica supported Pt nanocatalyst through a multi-carboxyl linker: synthesis, characterization, and applications in alkene hydrosilylation
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A magnetically recyclable superparamagnetic silica supported Pt nanocatalyst through a multi-carboxyl linker: synthesis, characterization, and applications in alkene hydrosilylation

机译:可磁循环的超顺磁性二氧化硅负载的Pt纳米催化剂通过多羧基连接基的合成,表征及其在烯烃氢化硅烷化中的应用

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摘要

To simplify separation procedures, improve the reusability and decrease the loss of Pt, two Pt catalysts anchored on superparamagnetic silica (Fe _(3) O _(4) @SiO _(2) -EDTA@Pt and Fe _(3) O _(4) @SiO _(2) -DTPA@Pt) were prepared for the first time. The stable magnetic properties made them easily recyclable using a magnet rather than filtration, decantation or centrifugation. After 12 catalytic runs for both 30–50 nm Pt catalysts, the yield of 1-heptylmethyldichlorosilane was still up to 90%. The average loss of Pt in each reaction was only 0.87% for Fe _(3) O _(4) @SiO _(2) -EDTA@Pt and 0.66% for Fe _(3) O _(4) @SiO _(2) -DTPA@Pt owing to the strong interaction between Pt and carboxyl. The unprecedented activity and selectivity of the two Pt nanoparticle catalysts were observed in the hydrosilylation of alkenes. The turnover number in the reaction between 1-hexene and methyldichlorosilane using 5 × 10 ~(?8) mol of the Pt approached 662?733 for Fe _(3) O _(4) @SiO _(2) -EDTA@Pt and 579?947 for Fe _(3) O _(4) @SiO _(2) -DTPA@Pt over 12 h. The corresponding hydrosilylation products in excellent yields were obtained when we employed a broad range of alkenes as substrates, including 5 isomerous hexenes and 14 important industry raw materials. Fe _(3) O _(4) @SiO _(2) -DTPA@Pt showed a better activity. They have potential for catalyzing more reactions and replacing the current homogeneous Pt catalysts in industry.
机译:为了简化分离程序,提高可重复使用性并减少Pt的损失,将两种Pt催化剂固定在超顺磁性二氧化硅上(Fe _(3)O _(4)@SiO _(2)-EDTA @ Pt和Fe _(3)O首次制备了_(4)@SiO_(2)-DTPA @ Pt)。稳定的磁性使它们易于使用磁铁而不是过滤,倾析或离心回收。在两种30–50 nm Pt催化剂上进行12次催化运行后,1-庚基甲基二氯硅烷的收率仍高达90%。 Fe _(3)O _(4)@SiO _(2)-EDTA @ Pt在每个反应中Pt的平均损失仅为0.87%,Fe _(3)O _(4)@SiO _仅为0.66% (2)-DTPA @ Pt是由于Pt与羧基之间的强相互作用。在烯烃的氢化硅烷化中观察到两种Pt纳米粒子催化剂具有前所未有的活性和选择性。 Fe _(3)O _(4)@SiO _(2)-EDTA @ Pt在使用5×10〜(?8)摩尔Pt的1-己烯与甲基二氯硅烷之间的反应转换数接近662?733 Fe _(3)O _(4)@SiO _(2)-DTPA @ Pt在12 h内为579?947。当我们使用多种烯烃作为底物(包括5种异构己烯和14种重要的工业原料)时,可以得到高产率的相应氢化硅烷化产物。 Fe _(3)O _(4)@SiO _(2)-DTPA @ Pt表现出更好的活性。它们具有催化更多反应并取代目前工业上均相Pt催化剂的潜力。

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