An efficient heterogeneous catalyst based on highly dispersed Na7H2LaW10O36•32H2O nanoparticles on mesoporous silica for deep desulfurization
An efficient heterogeneous catalyst based on highly dispersed Na7H2LaW10O36•32H2O nanoparticles on mesoporous silica for deep desulfurization
复制标题
DOI：
10.1016/j.apcata.2013.06.030
复制
发表时间：
2013-09-10
影响因子：
5.5
通讯作者：
Song, Yu-Fei
中科院分区：
文献类型：
--
作者：
Chen, Yang;Zhao, Shen;Song, Yu-Fei
以Na 7 H2 LaW 10 O36为中心点，通过有机连接剂将LaW 10与氨基改性的介孔氧化硅分子筛进行化学锚定。用ICP-ES、FT-IR、N2吸附、UV-vis、MAS-NMR和HR-TEM等手段对催化剂进行了表征。结果表明，LaW_（10）纳米粒子高度分散在介孔氧化硅表面，在H_2O_2存在下，以（SiO_2/NH_3 ~+/LaW_（10））/[bmim] BF_4（bmim=1-丁基-3-甲基咪唑）为催化剂，在35 min内实现了二苯并噻吩的高效深度脱硫，转化率接近100%。在硫含量低至100 ppm的模拟油中，脱硫效果较好.放大实验表明，当硫含量为1000 ppm时，模型油的体积从5 mL增加到1000 mL，在45 min内可达到100%的脱硫率。此外，催化剂可重复使用10次以上，且催化效率不降低。据我们所知，以H2 O2为氧化剂的（SiO2/NH3+/LaW 10）/[bmim] BF 4催化剂体系在迄今为止报道的脱硫系统中具有巨大的实际应用潜力。(C)2013爱思唯尔有限公司版权所有。
A lanthanide-containing polyoxometalate of Na7H2LaW10O36 center dot 32H(2)O (LaW10) have been chemically anchored to the amino-modified mesoporous silica through an organic linker. The catalysts have been characterized by ICP-ES, FT-IR, N-2 sorption measurements, UV-vis, MAS-NMR, and HR-TEM. It is found that the LaW10, nanoparticles are highly dispersed on mesoporous silica, and the resulting catalysts show highly efficient deep desulfurization in only 35 min with almost 100% conversion of dibenzothiophene by using (SiO2/NH3+/LaW10)/[bmim]BF4 (bmim=1-butyl-3-methylimidazolium) in the presence of H2O2 as oxidant. Furthermore, deep desulfurization proceeds smoothly in model oil with S content as low as 100 ppm. A scaled-up experiment, in which the volume of model oil increases from 5 to 1000 mL with S content of 1000 ppm, indicates that almost 100% sulfur removal can be achieved in 45 min. Additionally, the catalyst could be recycled and reused at least ten times without any decrease of the catalytic efficiency. To the best of our knowledge, the (SiO2/NH3+/LaW10)/[bmim]BF4 catalyst system with H2O2 as oxidant exhibits great potential for practical application as desulfurization systems reported so far. (C) 2013 Elsevier B.V. All rights reserved.