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介孔硅负载纳米铜对燃料油中二苯并噻吩的快速可逆吸附。

Fast and reversible adsorption for dibenzothiophene in fuel oils with metallic nano-copper supported on mesoporous silica.

机构信息

Department of Biological and Chemical Engineering, Guangxi University of Science and Technology, City, Liuzhou, 545006, China.

CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian City, 116023, China.

出版信息

Environ Sci Pollut Res Int. 2021 Jan;28(3):2741-2752. doi: 10.1007/s11356-020-10715-1. Epub 2020 Sep 6.

Abstract

Dibenzothiophene (DBT) in fuel oils causes the release of toxic sulfur oxide gases, and it is necessary to remove DBT in fuels. Herein, metallic copper was loaded on SBA-15 mesoporous silica through simple reduction reactions for the preparation of DBT adsorbents. On an adsorbent with a copper loading of 0.3 wt%, adsorption equilibrium was achieved within 5 min, and a DBT removal rate of 90.4% was achieved. The adsorption isotherm agreed with a linear Freundlich model and adsorption capacity was 12.1 mg sulfur/g. Nano-sized copper particles were observed by TEM, indicating the size effect of copper particles in DBT adsorption. A broad band, corresponding to copper-sulfur coordination bonds, was observed at 300-600 cm in the Raman spectrum of DBT-doped adsorbent. Meanwhile, the band at 1233 cm corresponding to C = C (-S) bonds in DBT was shifted to 1229 cm in DBT adsorbed. XPS and Cu LMM XPS spectra proved that Cu(0) was oxidized by DBT sulfur during adsorption. Furthermore, Auger spectra verified that the adsorption of DBT on Cu(0) involved the formation of Cu(I) and Cu(II) species through coordination bonds. The adsorption capacity could be completely recovered via elution. This work sheds light on the removal of DBT in fuel oils with cost-effective efficient adsorbents.

摘要

燃料油中的二苯并噻吩(DBT)会释放出有毒的硫氧化物气体,因此需要将 DBT 从燃料中去除。本文通过简单的还原反应将金属铜负载到 SBA-15 介孔硅上,制备了 DBT 吸附剂。在铜负载量为 0.3wt%的吸附剂上,吸附平衡在 5 分钟内达到,DBT 的去除率达到 90.4%。吸附等温线符合线性 Freundlich 模型,吸附容量为 12.1mg 硫/g。TEM 观察到纳米尺寸的铜颗粒,表明铜颗粒在 DBT 吸附中的尺寸效应。在 DBT 掺杂吸附剂的拉曼光谱中,观察到 300-600cm 处对应铜-硫配位键的宽带。同时,DBT 中对应 C = C(-S)键的 1233cm 处的峰位移到了 DBT 吸附后的 1229cm 处。XPS 和 Cu LMM XPS 谱图证明,在吸附过程中,DBT 中的硫将 Cu(0)氧化。此外,俄歇能谱图证实了 DBT 通过配位键吸附在 Cu(0)上形成了 Cu(I)和 Cu(II)物种。吸附容量可以通过洗脱完全回收。这项工作为使用具有成本效益的高效吸附剂去除燃料油中的 DBT 提供了思路。

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