An efficient heterogeneous catalyst based on highly dispersed Na7H2LaW10O36•32H2O nanoparticles on mesoporous silica for deep desulfurization

被引:45
作者
Chen, Yang [1 ]
Zhao, Shen [1 ]
Song, Yu-Fei [1 ]
机构
[1] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
基金
美国国家科学基金会;
关键词
Polyoxometalates; Desulfurization; Lanthanides; Mesoporous silica; IONIC LIQUIDS; OXIDATIVE DESULFURIZATION; ROOM-TEMPERATURE; POLYOXOMETALATE; EXTRACTION; DIESEL; FUELS; NANOSCALE; COMPLEXES; SYSTEMS;
D O I
10.1016/j.apcata.2013.06.030
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:307 / 314
页数:8
相关论文
共 27 条
  • [1] Selective oxidation of anthracene using inorganic-organic hybrid materials based on molybdovanadophosphoric acids
    Bordoloi, Ankur
    Lefebvre, E.
    Halligudi, S. B.
    [J]. JOURNAL OF CATALYSIS, 2007, 247 (02) : 166 - 175
  • [2] Desulfurization by oxidation combined with extraction using acidic room-temperature ionic liquids
    Chi Yansheng
    Li Changping
    Jiao Qingzhu
    Liu Qingshan
    Yan Peifang
    Liu Xiumei
    Welz-Biermann, Urs
    [J]. GREEN CHEMISTRY, 2011, 13 (05) : 1224 - 1229
  • [3] From serendipity to design of polyoxometalates at the nanoscale, aesthetic beauty and applications
    Cronin, Leroy
    Mueller, Achim
    [J]. CHEMICAL SOCIETY REVIEWS, 2012, 41 (22) : 7333 - 7334
  • [4] Ionic liquids on desulfurization of fuel oils
    Francisco, Maria
    Arce, Alberto
    Soto, Ana
    [J]. FLUID PHASE EQUILIBRIA, 2010, 294 (1-2) : 39 - 48
  • [5] Desulfurization and denitrogenation of gasoline and diesel fuels by means of ionic liquids
    Hansmeier, Antje R.
    Meindersma, G. Wytze
    de Haan, Andre B.
    [J]. GREEN CHEMISTRY, 2011, 13 (07) : 1907 - 1913
  • [6] Introduction: Polyoxometalates - Multicomponent molecular vehicles to probe fundamental issues and practical problems
    Hill, CL
    [J]. CHEMICAL REVIEWS, 1998, 98 (01) : 1 - 2
  • [7] Horniakova J, 2004, J MOL CATAL A-CHEM, V217, P73, DOI 10.1016/j.molcata.2004.02.019
  • [8] Heteropolyanion-Based Ionic Liquid for Deep Desulfurization of Fuels in Ionic Liquids
    Huang, Wangli
    Zhu, Wenshuai
    Li, Huaming
    Shi, Hua
    Zhu, Guopeng
    Liu, Hui
    Chen, Guangying
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (19) : 8998 - 9003
  • [9] Surface modification of mesoporous, macroporous, and amorphous silica with catalytically active polyoxometalate clusters
    Johnson, BJS
    Stein, A
    [J]. INORGANIC CHEMISTRY, 2001, 40 (04) : 801 - 808
  • [10] Deep desulfurization of diesel fuel using ionic liquids: current status and future challenges
    Kulkarni, Prashant S.
    Afonso, Carlos A. M.
    [J]. GREEN CHEMISTRY, 2010, 12 (07) : 1139 - 1149