Seed-mediated growth of MOF-encapsulated Pd@Ag core-shell nanoparticles: toward advanced room temperature nanocatalysts.
Seed-mediated growth of MOF-encapsulated Pd@Ag core-shell nanoparticles: toward advanced room temperature nanocatalysts.
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种子介导的MOF包含的PD@Ag核壳纳米颗粒的生长：朝向晚期室温纳米催化剂。
DOI：
10.1039/c5sc02925b
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发表时间：
2016-01-01
期刊：
影响因子：
8.4
通讯作者：
Li Y
中科院分区：
文献类型：
--
作者：
Chen L;Huang B;Qiu X;Wang X;Luque R;Li Y
以活化氢原子为还原剂，采用种子生长法在金属有机薄膜的孔内形成了核壳结构的Pd@Ag纳米粒子，从而得到了一类在室温反应中具有优异催化性能的多核壳结构金属有机薄膜纳米材料。本研究尝试利用金属有机骨架（MOFs）内的空腔作为模板制备微小的金属纳米粒子（NPs）。报道了通过种子介导的生长策略在MOF上的Pd@Ag核-壳NPs的前所未有的设计，并且归因于在嵌入的Pd NPs上存在活化的物理吸附的氢原子作为还原剂以选择性地引导Ag沉积到Pd上，同时使Ag自成核最小化。由于表面稀释和电子修饰的表面钯网站的Ag沉积，所获得的Pd@Ag核-壳纳米粒子表现出显着增加的选择性，在苯乙炔的部分氢化相比，其monopoly的同行，由于表面稀释和电子修饰。Pd@Ag纳米颗粒在催化反应中也具有前所未有的高稳定性和可回收性，这与纳米限制效应和MOF框架提供的强金属-载体相互作用有关。
Core–shell Pd@Ag nanoparticles are formed within the pores of MOFs via a seed mediated growth strategy with activated hydrogen atoms as the reducing agent, leading to a family of bimetallic core–shell MOF nanomaterials with excelling catalytic performance in room temperature reactions. The possibility of using inner cavities within metal–organic frameworks (MOFs) as templates for the fabrication of tiny metal nanoparticles (NPs) was attempted in this work. An unprecedented design of Pd@Ag core–shell NPs on MOFs via a seed mediated growth strategy is reported and attributed to the presence of activated physisorbed hydrogen atoms on embedded Pd NPs as reducing agents to selectively direct the deposition of Ag onto Pd while minimizing the Ag self-nucleation. The obtained Pd@Ag core–shell NPs exhibited a significant increase in selectivity in the partial hydrogenation of phenylacetylene as compared to their monometallic counterparts, due to the surface dilution and electron modification of the surface Pd sites by Ag deposition. Pd@Ag NPs also possessed an unprecedented high stability and recyclability in the catalytic reactions, related to the nano-confinement effect and the strong metal–support interaction offered by the MOF framework.
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