beta-Cyclodextrin polymer networks stabilized gold nanoparticle with superior catalytic activities
beta-Cyclodextrin polymer networks stabilized gold nanoparticle with superior catalytic activities
复制标题
β-环糊精聚合物网络稳定的金纳米粒子具有优异的催化活性
DOI：
10.1007/s12274-020-3144-7
复制
发表时间：
2021
期刊：
影响因子：
9.9
通讯作者：
Ding S.-Y.
中科院分区：
文献类型：
--
作者：
Zhang Y.;Hu B.;Cao X.-M.;Luo L.;Xiong Y.;Wang Z.-P.;Hong X.;Ding S.-Y.
载体材料在非均相纳米催化中起着重要的作用。在这项工作中，β-环糊精（β-CD）直接作为单体构建了用于金纳米颗粒（Au NPs）固定的聚合物网络。通过简单的亲核取代反应，成功制备了β-CD基聚合物网络（β-CDP-N和β- cdp - c）。与β- cdp - c相比，β- cdp -N中的羟基和N原子在固定较小的Au NPs方面发挥协同作用，从而具有较高的催化活性。值得注意的是，Au@β- cdp -n将4-硝基苯酚还原为4-氨基苯酚的表观速率常数（Kapp）值为14.15 × 10−2s−1，与之前报道的具有固体载体的Au NPs相比，在类似条件下有了显著的改善。考虑到β- cdp - n载体的孔隙率可以忽略不计，我们采用“捕获-催化-释放”模型来解释Au@β-CDP-N的高催化活性。这一解释得到了β- cdp - n的客体响应特性的支持。此外，Au@β-CDP-N易于回收，并且在7次成功循环后保持了较高的催化效率。
Support materials play a significant role in heterogeneous nanocatalysis. In this work,β-cyclodextrin (β-CD) was used directly as a monomer to construct polymer networks for gold nanoparticles (Au NPs) immobilization. Using the simple nucleophilic substitution reaction,β-CD based polymer networks (β-CDP-N andβ-CDP-C) were successfully prepared. Compared toβ-CDP-C, the hydroxyl groups and N atoms inβ-CDP-N played a synergistic role in immobilizing smaller Au NPs, thus leading to high catalytic activities. Notably, the apparent rate constant (Kapp) value for Au@β-CDP-N in the reduction of 4-nitrophenol to 4-aminophenol is 14.15 × 10−2s−1, which shows a significant improvement over all previously reported Au NPs with solid supports under similar conditions. Considering the negligible porosity of theβ-CDP-N support, we purposed a “capture-catalysis-release” model to explain the high catalytic activity of Au@β-CDP-N. This explanation is supported by the guest-responsive properties ofβ-CDP-N. Moreover, the Au@β-CDP-N is easily recycled and maintained its high catalytic efficiency after seven successful cycles.