Morphology Effect of Metal-organic Framework HKUST-1 as a Catalyst on Benzene Oxidation

doi:10.1007/s40242-017-6468-4

Abstract

Abstract: An attempt was made to study whether the morphology effect of metal-organic frameworks HKUST-1 could significantly influence the chemical reaction of benzene oxidation. Four representative cupric salts, CuSO₄·5H₂O, Cu(OAc)₂·H₂O, CuCl₂·2H₂O and Cu(NO₃)₂·3H₂O, were treated with 1,3,5-benzenetricarboxylic acid under ultrasound or with static method at room temperature to prepare metal-organic frameworks(12 types of HKUST-1 samples). And the as-prepared HKUST-1 materials were comprehensively investigated by X-ray diffraction, scanning electron microscopy and N₂ adsorption-desorption. The HKUST-1 samples with different morphologies and characterisitcs were employed as catalysts for benzene oxidation with H₂O₂ as oxidant at 60℃ in acetonitrile to achieve the aromatic oxygenates and test their yields. In all the HKUST-1 samples, the HKUST-1/SA, HKUST-1/SA0 and HKUST-1/UN had the higher catalytic activities with the yields of benzene oxygenates of 15.9%, 16.6% and 11.7%, respectively, which can be ascribed to the larger pore volume, the stronger benzene adsorption and the smaller fine crystal particles. Comparatively, the HKUST-1/SN0 and HKUST-1/SC0 with more intact crystal, larger surface area, lower pore volume and weaker benzene adsorption had the lower catalytic activities with the yields of benzene oxygenates not more than 4%. Therefore, our results confirmed that employing various cupric precursors to prepare the HKUST-1 samples with different morphologies and characteristics can be considered as a worth strategy to design many more powerful heterogeneous catalysts.

Key words: HKUST-1, Metal-organic framework, Morphology effect, Catalytic reaction, Benzene

LIU Yanfeng, LIU Boliang, ZHOU Qingfeng, ZHANG Tianyong, WU Wubin. Morphology Effect of Metal-organic Framework HKUST-1 as a Catalyst on Benzene Oxidation[J]. Chemical Research in Chinese Universities, 2017, 33(6): 971-978.

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