摘要
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＇ 5H20, Cu（OAc）a-H20, CuCI2.2H20 and Cu（NO3）2 3H20, were treated with 1,3,5-benzenetricarboxylic acid under ultrasound or with static method at room temperature to prepare metal-organic frarneworks（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 fme 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 confumed 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.
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＇ 5H20, Cu（OAc）a-H20, CuCI2.2H20 and Cu（NO3）2 3H20, were treated with 1,3,5-benzenetricarboxylic acid under ultrasound or with static method at room temperature to prepare metal-organic frarneworks（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 fme 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 confumed 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.
基金
Supported by the Natural Science Foundation of Haman Province, China（No.213010） and the Natural Science Foundation of Haman University, China（No. kyqd1612）.
