Chemical Vapor Deposition of Pd(C3H5)(C5H5) to Synthesize Pd@MOF-5 Catalysts for Suzuki Coupling Reaction
Chemical Vapor Deposition of Pd(C3H5)(C5H5) to Synthesize Pd@MOF-5 Catalysts for Suzuki Coupling Reaction
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DOI：
10.1007/s10562-012-0767-7
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发表时间：
2012-01
影响因子：
2.8
通讯作者：
Mingming Zhang;J. Guan;Bingsen Zhang;Dangsheng Su;C. Williams;Changhai Liang
中科院分区：
文献类型：
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作者：
Mingming Zhang;J. Guan;Bingsen Zhang;Dangsheng Su;C. Williams;Changhai Liang
摘要采用金属有机化学气相沉积（MOCVD）法在多孔金属有机骨架材料MOF-5上负载金属有机化合物[Pd（C3 H5）（C5 H5）]。采用粉末X射线衍射（PXRD）、傅里叶变换红外光谱（FT-IR）和固体核磁共振（NMR）对包合物[Pd（C3 H5）（C5 H5）]@MOF-5进行了表征。发现M0 F-5的主体晶格在前体插入后保持完整。由于钯与MOF-5中的苯二甲酸连接基之间的相互作用，前体中的-C3 H5配体更容易丢失，这为前体吸附的不可逆性提供了可能的解释。通过在室温下氢解包合化合物[Pd（C3 H5）（C5 H5）]@MOF-5，在MOF-5的空腔内形成尺寸约2-5 nm的Pd纳米颗粒。所得材料的N2吸附证实保留了高表面积。在Suzuki偶联反应中，Pd@M0F-5材料在第一次催化运行中显示出良好的活性。PXRD结果表明，在随后的反应中，MOF-5的晶体结构被完全破坏，导致活性大幅度下降。图摘要采用MOCVD方法成功地将钯纳米粒子嵌入到金属有机骨架MOF-5中，并将其用作Suzuki反应的催化剂。所制备的Pd@MOF-5具有非常高的BET表面积，其中Pd颗粒的尺寸为2-5 nm。将Pd@MOF-5用作Suzuki偶联反应的非均相催化剂，并获得了良好的活性。
AbstractThe highly porous metal organic framework MOF-5 was loaded with the metal–organic compound [Pd(C3H5)(C5H5)] by metal–organic chemical vapor deposition (MOCVD) method. The inclusion compound [Pd(C3H5)(C5H5)]@MOF-5 was characterized by powder X-ray diffraction (PXRD), Fourier-transform infrared (FT-IR) spectroscopy, and solid-state nuclear magnetic resonance spectroscopy. It was found that the host lattice of MOF-5 remained intact upon precursor insertion. The –C3H5ligand in the precursor is easier to lose due to the interaction between palladium and the benzenedicarboxylate linker in MOF-5, providing a possible explanation for the irreversibility of the precursor adsorption. Pd nanoparticles of about 2–5 nm in size was formed inside the cavities of MOF-5 by hydrogenolysis of the inclusion compound [Pd(C3H5)(C5H5)]@MOF-5 at room temperature. N2sorption of the obtained material confirmed that high surface area was retained. In the Suzuki coupling reaction the Pd@MOF-5 materials showed a good activity in the first catalytic run. However, the crystal structure of MOF-5 was completely destroyed during the following reaction runs, as confirmed by PXRD, which caused a big loss of the activity.Graphical AbstractThe embedding of palladium nanoparticles into the metal organic framework MOF-5 has been successfully prepared by MOCVD method, and been used as catalyst for Suzuki reaction. The prepared Pd@MOF-5 had a very high BET surface area with Pd particles in size of 2–5 nm. The Pd@MOF-5 was used as a heterogeneous catalyst for the Suzuki coupling reaction and achieved a good activity.