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以糖衍生的碳材料负载的氧化钴将乙苯绿色高效催化氧化为苯乙酮

Green and efficient catalytic oxidation of ethylbenzene to acetophenone over cobalt oxide supported on a carbon material derived from sugar.

作者信息

Li Jinhong, Song Zhimei, Cui Kaikai, Li Haonan, Han Mei, Wang Jinge, Chen Lidong

机构信息

School of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian, Liaoning, 110629, P. R. China.

BEFAR GROUP CO., LTD, Binzhou, Shandong, 256600, P. R. China.

出版信息

Phys Chem Chem Phys. 2024 Oct 9;26(39):25688-25696. doi: 10.1039/d4cp02803a.

DOI:10.1039/d4cp02803a
PMID:39351792
Abstract

The use of biomass as a carbon source to support metal oxides has significant advantages in environmental protection and reducing the cost of the catalyst. The critical point lies on the development of highly active and recyclable catalysts. In this study, sugar was used as a carbon source, and cobalt oxide was loaded an method and an impregnation method to prepare the catalyst, respectively. The catalysts were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) spectroscopy, Raman, electron paramagnetic resonance ( EPR) and N adsorption-desorption. The characterization results show that the macroporous carbon-supported cobalt oxide catalyst prepared by the method contains CoO nanoparticles on the support, but the dispersion of cobalt oxide on the support is more uniform compared with the catalyst prepared by the impregnation method. The catalytic performance of the prepared catalyst was evaluated through the oxidation of ethylbenzene (EB) to acetophenone (AP) as a probe reaction. Under the optimized reaction conditions, temperature () = 80 °C, (catalyst) : (EB) = 0.15, (HO) : (EB) : (KBr) = 14.4 : 1 : 0.1, = 8 h, and (EB) : (CHCOOH) = 1 : 10, the conversion of EB and the selectivity of AP were 84.1% and 81.3%, respectively. CoO/SC-10- exhibits improved reactivity of EB oxidation owing to cobalt ions on the carbon support that promote the free radical and acid catalytic reaction pathway. The cobalt oxide catalyst supported by biomass carbon has decent recycling and regeneration ability, which provides a new idea for the application of biomass.

摘要

将生物质作为碳源来负载金属氧化物在环境保护和降低催化剂成本方面具有显著优势。关键在于开发高活性和可循环使用的催化剂。在本研究中,以糖作为碳源,分别采用 法和浸渍法负载氧化钴来制备催化剂。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、高分辨率透射电子显微镜(HRTEM)、X 射线粉末衍射(XRD)、X 射线光电子能谱(XPS)、傅里叶变换红外(FT-IR)光谱、拉曼光谱、电子顺磁共振(EPR)和 N2 吸附-脱附对催化剂进行了表征。表征结果表明,采用 法制备的大孔碳负载氧化钴催化剂在载体上含有 CoO 纳米颗粒,但与浸渍法制备的催化剂相比,氧化钴在载体上的分散更均匀。通过以乙苯(EB)氧化为苯乙酮(AP)作为探针反应来评价所制备催化剂的催化性能。在优化的反应条件下,温度()= 80 °C,(催化剂)∶(EB)= 0.15,(H2O)∶(EB)∶(KBr)= 14.4∶1∶0.1, = 8 h,且(EB)∶(CH3COOH)= 1∶10 时,EB 的转化率和 AP 的选择性分别为 84.1%和 81.3%。由于碳载体上的钴离子促进了自由基和酸催化反应途径,CoO/SC-10-表现出改进的 EB 氧化反应活性。生物质碳负载的氧化钴催化剂具有良好的循环和再生能力,这为生物质的应用提供了新思路。

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