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用于二苯并噻吩氧化脱硫的高效可重复使用的有序介孔WO /SnO催化剂

Efficient and reusable ordered mesoporous WO /SnO catalyst for oxidative desulfurization of dibenzothiophene.

作者信息

Piao Wenxiang, Li Zhenghua, Li Chengbin, Park Jin Seo, Lee Jung-Ho, Li Zhengyang, Kim Ki Yeong, Jin Long Yi, Kim Ji Man, Jin Mingshi

机构信息

Department of Chemistry Park Road 977 Yanji City Jilin Province 133002 P. R. China

Department of Chemistry, Sungkyunkwan University Suwon 440-746 Republic of Korea.

出版信息

RSC Adv. 2021 Aug 13;11(44):27453-27460. doi: 10.1039/d1ra04957g. eCollection 2021 Aug 9.

Abstract

The oxidative desulfurization (ODS) of organic sulfur compounds over tungsten oxide supported on highly ordered mesoporous SnO (WO /meso-SnO) was investigated. A series of WO /meso-SnO with WO contents from 10 wt% to 30 wt%, were prepared by conventional wet impregnation. The physico-chemical properties of the WO /meso-SnO catalysts were characterized by X-ray diffraction (XRD), N adsorption-desorption isotherms, electron microscopy, Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy, and the temperature-programmed reduction of hydrogen (H-TPR). The characterization results indicated that these catalysts possessed mesoporous structures with uniform pores, high specific surface areas, and well-dispersed polyoxotungstate species on the surface of meso-SnO support. The ODS performances were evaluated in a biphasic system (model oil/acetonitrile, = 2000 ppm), using HO as an oxidant, and acetonitrile as an extractant. Dibenzothiophene (DBT) in the model oil was removed completely within 60 min at 50 °C using 20 wt% WO /meso-SnO catalyst. Additionally, the effect of reaction temperature, HO/DBT molar ratio, amount of catalyst and different sulfur-containing substrates on the catalytic performances were also investigated in detail. More importantly, the 20 wt% WO /meso-SnO catalyst exhibited 100% surfur-removal efficiency without any regeneration process, even after six times recycling.

摘要

研究了负载在高度有序介孔SnO上的氧化钨(WO /介孔SnO)对有机硫化合物的氧化脱硫(ODS)性能。采用传统的湿浸渍法制备了一系列WO 含量为10 wt%至30 wt%的WO /介孔SnO。通过X射线衍射(XRD)、N吸附-脱附等温线、电子显微镜、傅里叶变换红外光谱(FT-IR)、拉曼光谱以及氢气程序升温还原(H-TPR)对WO /介孔SnO催化剂的物理化学性质进行了表征。表征结果表明,这些催化剂具有介孔结构,孔径均匀,比表面积高,且多金属氧酸盐物种在介孔SnO载体表面分散良好。在双相体系(模型油/乙腈, = 2000 ppm)中,以HO作为氧化剂,乙腈作为萃取剂,对ODS性能进行了评估。使用20 wt%的WO /介孔SnO催化剂,在50 °C下60分钟内可将模型油中的二苯并噻吩(DBT)完全去除。此外,还详细研究了反应温度、HO/DBT摩尔比、催化剂用量以及不同含硫底物对催化性能的影响。更重要的是,即使经过六次循环,20 wt%的WO /介孔SnO催化剂在无需任何再生过程的情况下仍表现出100%的脱硫效率。

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