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以过氧化氢为氧化剂,坡缕石负载α-MnO纳米片催化二苯并噻吩的氧化脱硫

Oxidative desulfurization of dibenzothiophene catalyzed by α-MnO nanosheets on palygorskite using hydrogen peroxide as oxidant.

作者信息

Yu Xingming, Han Pingfang, Li Ya

机构信息

Biotechnology and Pharmaceutical Engineering, Nanjing Tech University Nanjing P. R. China

Nantong College of Science and Technology Nantong 226007 P. R. China.

出版信息

RSC Adv. 2018 May 16;8(32):17938-17943. doi: 10.1039/c8ra02396d. eCollection 2018 May 14.

DOI:10.1039/c8ra02396d
PMID:35542101
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9080502/
Abstract

Palygorskite (Pal)-supported α-MnO nanosheets (Ns-MnPal) combine the adsorption features of Pal with the catalytic properties of α-MnO nanosheets. They were prepared and examined in the catalytic oxidative desulfurization (ODS) of dibenzothiophene (DBT) from a model oil employing 30 wt% HO as the oxidant under mild conditions. The supported catalyst was fabricated by the solvothermal method, and effective immobilization of α-MnO nanosheets was confirmed by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS) and N adsorption. The influence of various solvents, solvent volume, reaction temperature, reaction time, catalyst amount and HO/sulfur molar ratio on ODS was investigated. Using 20 mL of acetonitrile as a solvent, maximum sulfur removal of 97.7% was achieved for ODS of DBT in 1.5 h using a Ns-MnPal/oil ratio of 0.2 g L, reaction temperature of 50 °C and HO/sulfur molar ratio of 4. As solid catalysts, supported α-MnO nanosheets could be separated from the reaction readily. The catalyst was recycled seven times and showed no significant loss in activity.

摘要

坡缕石(Pal)负载的α-MnO纳米片(Ns-MnPal)结合了坡缕石的吸附特性和α-MnO纳米片的催化性能。在温和条件下,以30 wt%的H₂O₂作为氧化剂,对模拟油中二苯并噻吩(DBT)的催化氧化脱硫(ODS)反应进行了制备和研究。通过溶剂热法制备了负载型催化剂,并通过X射线衍射(XRD)、扫描电子显微镜(SEM)、能谱分析(EDS)、热重分析(TGA)、X射线光电子能谱(XPS)和N₂吸附等方法证实了α-MnO纳米片的有效负载。研究了各种溶剂、溶剂体积、反应温度、反应时间、催化剂用量和H₂O₂/硫摩尔比对ODS的影响。以20 mL乙腈为溶剂,在Ns-MnPal/油比为0.2 g L⁻¹、反应温度为50℃、H₂O₂/硫摩尔比为4的条件下,1.5 h内DBT的ODS反应最大脱硫率达到97.7%。作为固体催化剂,负载的α-MnO纳米片可很容易地从反应体系中分离出来。该催化剂循环使用了7次,活性没有明显损失。

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