Abstract
Highly ordered three-dimensional (3DOM) macroporous polyoxometalate (POM)-based zirconia hybrids with relatively high surface area and interconnected pore structure have been fabricated by colloidal crystal template method. Owing to the evenly distributed POM active sites, large-scaled 3D ordered macroporous structure, and high porosity of as-synthesized POM-based ZrO2 composite, it exhibits excellent extractive-oxidative desulfurization activity and recyclability. 500 ppm of dibenzothiophene (DBT) in the model fuel can be removed within 2 h under mild conditions and no obvious loss of catalytic activity even after 20 times. The oxidative reaction of DBT follows pseudo-first-order kinetics, corresponded to an Arrhenius activation energy of 61.1 kJ/mol.
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V. Hulea, F. Fajula, J. Bousquet, Mild oxidation with H2O2 over Ti-containing molecular sieves - A very efficient method for removing aromatic sulfur compounds from fuels. J. Catal. 198(2), 179–186 (2001)
J. Xiao, S. Sitamraju, Y.S. Chen et al., Air-promoted adsorptive desulfurization of diesel fuel over Ti-Ce mixed metal oxides. AICHE J. 61(2), 631–639 (2015)
G. Ye, Y. Gu, W. Zhou et al., Synthesis of defect-rich titanium terephthalate with the assistance of acetic acid for room-temperature oxidative desulfurization of fuel oil. ACS Catal. 10(3), 2384–2394 (2020)
Y. Gu, G. Ye, W. Xu et al., Creation of active sites in MOF-808(Zr) by a facile route for oxidative desulfurization of model diesel oil. Chemistryselect 5(1), 244–251 (2020)
M. Taghizadeh, E. Mehrvarz, A. Taghipour, Polyoxometalate as an effective catalyst for the oxidative desulfurization of liquid fuels: a critical review. Rev. Chem. Eng. (2020). https://doi.org/10.1515/revce-2018-0058
A. Akbari, M. Chamack, M. Omidkhah, Reverse microemulsion synthesis of polyoxometalate-based heterogeneous hybrid catalysts for oxidative desulfurization. J. Mater. Sci. 55(15), 6513–6524 (2020)
B. Wang, B. Dai, L. Kang et al., Synthesis of three-dimensional ordered mesoporous W-doped KIT-6 for oxidative desulfurization catalyst of fuels. Fuel (2020). https://doi.org/10.1016/j.fuel.2020.117029
J. Xiong, J. Luo, J. Di et al., Macroscopic 3D boron nitride monolith for efficient adsorptive desulfurization. Fuel (2020). https://doi.org/10.1016/j.fuel.2019.116448
Z.C. Kampouraki, D.A. Giannakoudakis, K.S. Triantafyllidis et al., Catalytic oxidative desulfurization of a 4,6-DMDBT containing model fuel by metal-free activated carbons: the key role of surface chemistry. Green Chem. 21(24), 6685–6698 (2019)
W. Xiao, Q. Dong, Y. Wang et al., Time modulation of defects in UiO-66 and application in oxidative desulfurization. CrystEngComm 20(38), 5658–5662 (2018)
S. Xun, C. Hou, H. Li et al., Synthesis of WO3/mesoporous ZrO2 catalyst as a high-efficiency catalyst for catalytic oxidation of dibenzothiophene in diesel. J. Mater. Sci. 53(23), 15927–15938 (2018)
B. Liu, R.T. Baker, Factors affecting the preparation of ordered mesoporous ZrO2 using the replica method. J. Mater. Chem. 18(43), 5200–5207 (2008)
E. Torres-García, A. Galano, G. Rodriguez-Gattorno, Oxidative desulfurization (ODS) of organosulfur compounds catalyzed by peroxo-metallate complexes of WOx-ZrO2: Thermochemical, structural, and reactivity indexes analyses. J. Catal. 282(1), 201–208 (2011)
Z. Hasan, J. Jeon, S.H. Jhung, Oxidative desulfurization of benzothiophene and thiophene with WOx/ZrO2 catalysts: Effect of calcination temperature of catalysts. J. Hazard. Mater. 205–206, 216–221 (2012)
G. Rodriguez-Gattorno, A. Galano, E. Torres-García, Surface acid-basic properties of WOx-ZrO2 and catalytic efficiency in oxidative desulfurization. Appl. Catal. B 92(1–2), 1–8 (2009)
Y. Du, J. Lei, Y. Peng et al., Three-dimensional ordered phosphotungstic acid/TiO2 with superior catalytic activity for oxidative desulfurization. Fuel 226, 148–155 (2018)
Y. Du, P. Yang, S. Zhou et al., Direct synthesis of ordered meso/macrostructured phosphotungstic acid/SiO2 by EISA method and its catalytic performance of fuel oil. Mater. Res. Bull. 97, 42–48 (2018)
Y. Du, L. Jiaheng, Z. Lina et al., Highly efficient deep desulfurization of fuels by meso/macroporous H3PW12O40/TiO2 at room temperature. Mater. Res. Bull. 105, 210–219 (2018)
C.D. Dushkin, G.S. Lazarov, S.N. Kotsev et al., Effect of growth conditions on the structure of two-dimensional latex crystals: experiment. Colloid Polym. Sci. 277(10), 914–930 (1999)
D. Yue, J. Lei, Z. Lina et al., Three-dimensional ordered macroporous HPW/titania-alumina catalysts for catalytic oxidative desulfurization of fuels. J. Porous Mater. 26(1), 133–144 (2019)
E. Torres-Garcia, A. Galano, G. Rodriguez-Gattorno, Oxidative desulfurization (ODS) of organosulfur compounds catalyzed by peroxo-metallate complexes of WOx-ZrO2: thermochemical, structural, and reactivity indexes analyses. J. Catal. 282(1), 201–208 (2011)
M. Zhang, J. Liu, J. Yang et al., Molybdenum-containing dendritic mesoporous silica spheres for fast oxidative desulfurization in fuel. Inorg. Chem. Front. 6(2), 451–458 (2019)
H.L. Fan, T. Sun, Y.P. Zhao et al., Three-dimensionally ordered macroporous iron oxide for removal of H2S at medium temperatures. Environ. Sci. Technol. 47(9), 4859–4865 (2013)
Y. Wang, Y. Zhang, H. Lu et al., Novel N-doped ZrO2 with enhanced visible-light photocatalytic activity for hydrogen production and degradation of organic dyes. RSC Adv. 8(13), 6752–6758 (2018)
X. Yan, Z. Mei, P. Mei et al., Self-assembled HPW/silica-alumina mesoporous nanocomposite as catalysts for oxidative desulfurization of fuel oil. J. Porous Mater. 21(5), 729–737 (2014)
X.M. Yan, P. Mei, L. Xiong et al., Mesoporous titania-silica-polyoxometalate nanocomposite materials for catalytic oxidation desulfurization of fuel oil. Catal. Sci. Technol. 3(8), 1985–1992 (2013)
Y. Wei, M. Zhang, P. Wu et al., Tailoring electronic properties of porphyrin manganese on boron nitride for enhancing aerobic oxidative desulfurization at room temperature. ACS Sustain. Chem. Eng. 8(2), 1015–1022 (2020)
X. Chen, M. Zhang, Y. Wei et al., Ionic liquid-supported 3DOM silica for efficient heterogeneous oxidative desulfurization. Inorg. Chem. Front. 5(10), 2478–2485 (2018)
S. Wei, H. He, Y. Cheng et al., Preparation, characterization, and catalytic performances of cobalt catalysts supported on KIT-6 silicas in oxidative desulfurization of dibenzothiophene. Fuel 200, 11–21 (2017)
J. Zhang, A.J. Wang, X. Li et al., Oxidative desulfurization of dibenzothiophene and diesel over [Bmim](3)PMo12O40[J]. J. Catal. 279(2), 269–275 (2011)
G. Estephane, C. Lancelot, P. Blanchard et al., W-SBA based materials as efficient catalysts for the ODS of model and real feeds: improvement of their lifetime through active phase encapsulation. Appl. Catal. 571, 42–50 (2019)
M. Zhang, Y. Wei, R. Li et al., Magnetic POM-based mesoporous silica for fast oxidation of aromatic sulfur compounds. Fuel 209, 545–551 (2017)
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This work was supported by the National Natural Science Foundation of China (No.51801059) and National Postdoctoral Program for Innovative Talents (BX20190258).
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Du, Y., Zhou, L., Liu, Z. et al. Polyoxometalate-based 3DOM ZrO2 material for deep oxidative desulfurization of DBT with ultrahigh stability. J Porous Mater 28, 109–116 (2021). https://doi.org/10.1007/s10934-020-00969-y
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DOI: https://doi.org/10.1007/s10934-020-00969-y