Temperature-dependent synthesis of Pd@ZIF-L catalysts via an assembly method

Temperature-dependent synthesis of Pd@ZIF-L catalysts via an assembly method
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通过组装方法随温度合成 Pd@ZIF-L 催化剂

DOI:
10.1016/j.micromeso.2017.02.007
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发表时间:
2017-05
影响因子:
5.2
通讯作者:
Rizhi Chen
Rizhi Chen
中科院分区:
材料科学2区
文献类型:
--
作者:
Hong Jiang;Songlin Xue;Yefei Liu;Weihong Xing;Rizhi Chen

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以二维层状咪唑骨架L型分子筛(ZIF-L)为载体,采用自组装法制备了十字星状、粒径约20 μm的Pd@ZIF-L催化剂。以对硝基苯酚对氨基苯酚的催化还原反应评价了它们的催化活性。结果表明,合成温度对Pd@ZIF-L催化剂的物理化学性质和催化性能有很大影响。温度的变化可以使催化剂从二维片状向零维球形转变。高温有利于增加Pd负载量并将Pd纳米颗粒包封在ZIF-L基质内。然而,在高于30 °C的温度下,形成致密的dia(Zn)结构。增加Pd@ZIF-L催化剂中的Pd负载导致显著更高的对硝基苯酚转化率。合成的催化剂结构相对致密,使得硝基苯酚难以进入活性中心,催化活性较低。这些发现将有助于开发高性能的Pd@ZIF-L催化剂。
The Pd@ZIF-L catalysts with uniform crosshair-star shape and a size of about 20 μm were synthesized by an assembly method, in which a two-dimensional layered zeolitic imidazolate framework-L (ZIF-L) was used as the support to immobilize Pd nanoparticles. Their catalytic activities were evaluated by the catalytic reduction ofp-nitrophenol top-aminophenol. The results highlight that the physical-chemical and catalytic properties of the Pd@ZIF-L catalysts are greatly affected by the synthesis temperature. The temperature variation can make the catalysts transform from two-dimensional flakes to zero-dimensional spheres. High temperature is beneficial for increasing Pd loading and encapsulating Pd nanoparticles within the ZIF-L matrix. However, under the temperature larger than 30 °C, the dense dia(Zn) structures are formed. Increasing Pd loading in the Pd@ZIF-L catalysts leads to a significantly higherp-nitrophenol conversion. The relative dense structure of the as-synthesized catalysts makesp-nitrophenol access the active centers difficultly and a lower catalytic activity is observed. These findings would aid the development of high-performance Pd@ZIF-L catalysts.
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