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

doi:10.1007/s40242-017-6468-4

高等学校化学研究 ›› 2017, Vol. 33 ›› Issue (6): 971-978.doi: 10.1007/s40242-017-6468-4

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

LIU Yanfeng¹, LIU Boliang^1,2, ZHOU Qingfeng¹, ZHANG Tianyong², WU Wubin²

1. School of Material and Chemical Engineering, Hainan University, Haikou 570228, P. R. China;
2. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, P. R. China

收稿日期:2016-11-23 修回日期:2017-01-13 出版日期:2017-12-01 发布日期:2017-04-17
通讯作者: ZHANG Tianyong,E-mail:tyzhang@tju.edu.cn E-mail:tyzhang@tju.edu.cn
基金资助:
Supported by the Natural Science Foundation of Hainan Province, China(No.213010) and the Natural Science Foundation of Hainan University, China(No. kyqd1612).

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

LIU Yanfeng¹, LIU Boliang^1,2, ZHOU Qingfeng¹, ZHANG Tianyong², WU Wubin²

1. School of Material and Chemical Engineering, Hainan University, Haikou 570228, P. R. China;
2. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, P. R. China

Received:2016-11-23 Revised:2017-01-13 Online:2017-12-01 Published:2017-04-17
Contact: ZHANG Tianyong,E-mail:tyzhang@tju.edu.cn E-mail:tyzhang@tju.edu.cn
Supported by:
Supported by the Natural Science Foundation of Hainan Province, China(No.213010) and the Natural Science Foundation of Hainan University, China(No. kyqd1612).

摘要/Abstract

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, CuSO₄·5H₂O, 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.

关键词: HKUST-1, Metal-organic framework, Morphology effect, Catalytic reaction, Benzene

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]. 高等学校化学研究, 2017, 33(6): 971-978.

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

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

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