Tuning the hydrogenation activity of Pd NPs on Al–MIL-53 by linker modification
Tuning the hydrogenation activity of Pd NPs on Al–MIL-53 by linker modification
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DOI：
10.1039/c3cy00910f
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发表时间：
2014-02
影响因子：
5
通讯作者：
Daming Zhang;Y. Guan;E. Hensen;Teng Xue;Yimeng Wang
中科院分区：
文献类型：
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作者：
Daming Zhang;Y. Guan;E. Hensen;Teng Xue;Yimeng Wang
3 wt.%的加氢活性研究了Pd纳米粒子负载在不同单基团（H、OCH 3、NH 2、Cl和NO 2）取代的Al-MIL-53材料上的情况。取代基增强了钯纳米粒子在Al-MIL-53上的分散，导致在2至4 nm范围内的窄粒度分布。在新鲜催化剂上的Pd纳米颗粒作为具有不同比率的Pd（II）和Pd（0）的混合物存在。即使在室温下，这些Pd物质在氢气流中也容易变成金属。它们对苯酚和苯乙炔的加氢活性与骨架芳环上的取代基有关。具有供电子基团（OCH 3和NH 2）的催化剂比具有吸电子基团（Cl和NO 2）的催化剂表现出更高的活性。这可能是由于有机连接体影响了金属Pd纳米粒子的氢解离能力。
The hydrogenation activity of 3 wt.% Pd nanoparticles supported on various mono-group (H, OCH3, NH2, Cl, and NO2) substituted Al–MIL-53 materials has been investigated. Substituents enhanced the dispersion of palladium nanoparticles on Al–MIL-53, leading to a narrow particle size distribution in the range of 2 to 4 nm. Pd nanoparticles on fresh catalysts were present as a mixture of Pd(II) and Pd(0) with different ratios. These Pd species readily became metallic in a hydrogen flow even at room temperature. Their activities in hydrogenation of phenol and phenylacetylene are linked to the substituents on the aromatic ring of the framework. Catalysts with electron-donating groups (OCH3 and NH2) show much higher activity than those containing electron-withdrawing groups (Cl and NO2). This behavior might be explained by the hydrogen dissociation abilities of metallic Pd nanoparticles affected by the organic linkers.