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Enhanced performances in catalytic oxidation of o-xylene over hierarchical macro-/mesoporous silica-supported palladium catalysts

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Abstract

A series of hierarchical macro-/mesoporous silica supports (MMSs) were successfully synthesized using dual-templating technique employing polystyrene (PS) spheres and the Pluronic P123 surfactant. Pd was next loaded on the hierarchical silica supports via colloids precipitation method. Physicochemical properties of the synthesized samples were characterized by various techniques and all catalysts were tested for the total oxidation of o-xylene. Among them, the Pd/MMS-b catalyst with tetraethoxysilane/polystyrene weight ratio of 1.0 exhibited superior catalytic activity, and under a higher gas hourly space velocity (GHSV) of 70000 h–1, the 90% conversion of o-xylene has been obtained at around 200°C. The BET and SEM results indicated that Pd/MMSb catalyst possesses high surface area and large pore volume, and well-ordered, interconnected macropores and 2D hexagonally mesopores hybrid network. This novel ordered hierarchical porous structure was highly beneficial to the dispersion of active sites Pd nanoparticles with less aggregation, and facilitates diffusion of reactants and products. Furthermore, the Pd/MMS-b catalyst possessed good stability and durability.

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References

  1. Huang Q, Xue X, Zhou R. Decomposition of 1,2-dichloroethane over CeO2 modified USY zeolite catalysts: effect of acidity and redox property on the catalytic behavior. Journal of Hazardous Materials, 2010, 183(1–3): 694–700

    Article  CAS  Google Scholar 

  2. Schottler M, Hottenroth H, Schluter B, Schmidt M. Volatile organic compound abatement in semiconductor and solar cell fabrication with respect to resource depletion. Chemical Engineering & Technology, 2010, 33(4): 638–646

    CAS  Google Scholar 

  3. Fang B, Kim J H, Kim M S, Yu J S. Hierarchical nanostructured carbons with meso-macroporosity: design, characterization, and applications. Accounts of Chemical Research, 2013, 46(7): 1397–1406

    Article  CAS  Google Scholar 

  4. Yao J M, ZhanWC, Liu X H, Guo Y L,Wang Y Q, Guo Y, Lu G Z. Catalytic performance of Ti-SBA-15 prepared by chemical vapor deposition for propylene epoxidation. Microporous and Mesoporous Materials, 2012, 148(1): 131–136

    Article  CAS  Google Scholar 

  5. Popova M, Szegedi A, Cherkezova-Zheleva Z, Mitov I, Kostova N, Tsoncheva T. Toluene oxidation on titanium- and iron-modified MCM-41 materials. Journal of Hazardous Materials, 2009, 168(1): 226–232

    Article  CAS  Google Scholar 

  6. Zhao W, Cheng J, Wang L N, Chu J L, Qu J K, Liu Y H, Li S H, Zhang H, Wang J C, Hao Z P, Qi T. Catalytic combustion of chlorobenzene on the Ln modified Co/HMS. Applied Catalysis B: Environmental, 2012, 127: 246–254

    Article  CAS  Google Scholar 

  7. Tsoncheva T, Issa G, Nieto J M L, Blasco T, Concepcion P, Dimitrov M, Atanasova G, Kovacheva D. Pore topology control of supported on mesoporous silicas copper and cerium oxide catalysts for ethyl acetate oxidation. Microporous and Mesoporous Materials, 2013, 180: 156–161

    Article  CAS  Google Scholar 

  8. He C, Li P, Wang H, Cheng J, Zhang X, Wang Y, Hao Z. Ligandassisted preparation of highly active and stable nanometric Pd confined catalysts for deep catalytic oxidation of toluene. Journal of Hazardous Materials, 2010, 181(1–3): 996–1003

    Article  CAS  Google Scholar 

  9. Bendahou K, Cherif L, Siffert S, Tidahy H L, Benaïssa H, Aboukaïs A. The effect of the use of lanthanum-doped mesoporous SBA-15 on the performance of Pt/SBA-15 and Pd/SBA-15 catalysts for total oxidation of toluene. Applied Catalysis A, 2008, 351(1): 82–87

    Article  CAS  Google Scholar 

  10. Ramanathan A, Subramaniam B, Maheswari R, Hanefeld U. Synthesis and characterization of Zirconium incorporated ultra large pore mesoporous silicate, Zr–KIT-6. Microporous and Mesoporous Materials, 2013, 167: 207–212

    Article  CAS  Google Scholar 

  11. Barbier J. Deactivation of reforming catalysts by coking–a review. Applied Catalysis, 1986, 23(2): 225–243

    Article  CAS  Google Scholar 

  12. Sun Z K, Deng Y H, Wei J, Gu D, Tu B, Zhao D Y. Hierarchically ordered macro-/mesoporous silica monolith: tuning macropore entrance size for size-selective adsorption of proteins. Chemistry of Materials, 2011, 23(8): 2176–2184

    Article  CAS  Google Scholar 

  13. Kim Y S, Guo X F, Kim G J. Asymmetric ring opening reaction of catalyst immobilized on silica monolith with bimodal meso/ macroscopic pore structure. Topics in Catalysis, 2009, 52(1–2): 197–204

    Article  CAS  Google Scholar 

  14. Du J, Lai X, Yang N, Zhai J, Kisailus D, Su F, Wang D, Jiang L. Hierarchically ordered macro-mesoporous TiO2-graphene composite films: improved mass transfer, reduced charge recombination, and their enhanced photocatalytic activities. ACS Nano, 2011, 5(1): 590–596

    Article  CAS  Google Scholar 

  15. Liu J, Li M, Wang J, Song Y, Jiang L, Murakami T, Fujishima A. Hierarchically macro-/mesoporous Ti-Si oxides photonic crystal with highly efficient photocatalytic capability. Environmental Science & Technology, 2009, 43(24): 9425–9431

    Article  CAS  Google Scholar 

  16. Dhainaut J, Dacquin J P, Lee A F, Wilson K. Hierarchical macroporous-mesoporous SBA-15 sulfonic acid catalysts for biodiesel synthesis. Green Chemistry, 2010, 12(2): 296–303

    Article  CAS  Google Scholar 

  17. Chiu J J, Pine D J, Bishop S T, Chmelka B F. Friedel–Crafts alkylation properties of aluminosilica SBA-15 meso/macroporous monoliths and mesoporous powders. Journal of Catalysis, 2004, 221 (2): 400–412

    Article  CAS  Google Scholar 

  18. Rudisill S G,Wang Z Y, Stein A. Maintaining the structure of templated porous materials for reactive and high-temperature applications. Langmuir, 2012, 28(19): 7310–7324

    Article  CAS  Google Scholar 

  19. Stein A, Wilson B E, Rudisill S G. Design and functionality of colloidal-crystal-templated materials—chemical applications of inverse opals. Chemical Society Reviews, 2013, 42(7): 2763–2803

    Article  CAS  Google Scholar 

  20. Zhao D Y, Huo Q S, Feng J L, Chemlka B F, Stucky G D. Nonionic triblock and star diblock copolymer and oligomeric surfactant syntheses of highly ordered, hydrothermally stable, mesoporous silica structures. Journal of the American Chemical Society, 1998, 120(24): 6024–6036

    Article  CAS  Google Scholar 

  21. Cao E, Sankar M, Nowicka E, He Q, Morad M, Miedziak P J, Taylor S H, Knight D W, Bethell D, Kiely C J, Gavriilidis A, Hutchings G J. Selective suppression of disproportionation reaction in solventless benzyl alcohol oxidation catalysed by supported Au–Pd nanoparticles. Catalysis Today, 2013, 203: 146–152

    Article  CAS  Google Scholar 

  22. Dou J, Zeng H C. Integrated networks of mesoporous silica nanowires and their bifunctional catalysis-sorption application for oxidative desulfurization. ACS Catalysis, 2014, 4(2): 566–576

    Article  CAS  Google Scholar 

  23. Deng WH, Toepke MW, Shanks B H. Surfactant-assisted synthesis of alumina with hierarchical nanopores. Advanced Functional Materials, 2003, 13(1): 61–65

    Article  CAS  Google Scholar 

  24. Yuan J, Dai H X, Zhang L, Deng J G, Liu Y X, Zhang H, Jiang H Y, He H. PMMA-templating preparation and catalytic properties of high-surface-area three-dimensional macroporous La2CuO4 for methane combustion. Catalysis Today, 2011, 175(1): 209–215

    Article  CAS  Google Scholar 

  25. Liu B C, Liu Y, Li C Y, Hu W T, Jing P, Wang Q, Zhang J. Three-dimensionally ordered macroporous Au/CeO2-Co3O4 catalysts with nanoporous walls for enhanced catalytic oxidation of formaldehyde. Applied Catalysis B: Environmental, 2012, 127: 47–58

    Article  CAS  Google Scholar 

  26. Yun J S, Ihm S K. Synthesis of mesoporous SBA-15 having macropores by dual-templating method. Journal of Physics and Chemistry of Solids, 2008, 69(5–6): 1133–1135

    Article  CAS  Google Scholar 

  27. Parlett C M A, Keshwalla P, Wainwright S G, Bruce D W, Hondow N S, Wilson K, Lee A F. Hierarchically ordered nanoporous Pd/ SBA-15 catalyst for the aerobic selective oxidation of sterically challenging allylic alcohols. ACS Catalysis, 2013, 3(9): 2122–2129

    Article  CAS  Google Scholar 

  28. Parlett C M A, Bruce D W, Hondow N S, Newton M A, Lee A F, Wilson K. Mesoporous silicas as versatile supports to tune the palladium-catalyzed selective aerobic oxidation of allylic alcohols. ChemCatChem, 2013, 5(4): 939–950

    Article  CAS  Google Scholar 

  29. Chen L F, González G, Wang J A, Noreña L E, Toledo A, Castillo S, Morán-Pineda M. Surfactant-controlled synthesis of Pd/Ce0.6Zr0.4O2 catalyst for NO reduction by CO with excess oxygen. Applied Surface Science, 2005, 243(1–4): 319–328

    Article  CAS  Google Scholar 

  30. Becker L, Forster H. Oxidative decomposition of benzene and its methyl derivatives catalyzed by copper and palladium ionexchanged Y-type zeolites. Applied Catalysis B: Environmental, 1998, 17(1–2): 43–49

    Article  CAS  Google Scholar 

  31. He C, Li J J, Cheng J, Li L D, Li P, Hao Z, Xu Z P. Ha Z P, Xu Z P. Comparative studies on porous material-supported Pd catalysts for catalytic oxidation of benzene, toluene, and ethyl acetate. Industrial & Engineering Chemistry Research, 2009, 48(15): 6930–6936

    Article  CAS  Google Scholar 

  32. Wang F, Li J S, Yuan J F, Sun X Y, Shen J Y, Han W Q, Wang L J. Short channeled Zr-Ce-SBA-15 supported palladium catalysts for toluene catalytic oxidation. Catalysis Communications, 2011, 12 (15): 1415–1419

    Article  CAS  Google Scholar 

  33. Pérez-Ramírez J, Christensen C H, Egeblad K, Christensen C H, Groen J C. Hierarchical zeolites: enhanced utilisation of microporous crystals in catalysis by advances in materials design. Chemical Society Reviews, 2008, 37(11): 2530–2542

    Article  Google Scholar 

  34. Kortunov P, Vasenkov S, Kärger J, Valiullin R, Gottschalk P, ElíaM F, Perez M, Stöcker M, Drescher B, McElhiney G, Berger C, Gläser R, Weitkamp J. The role of mesopores in intracrystalline transport in USY zeolite: PFG NMR diffusion study on various length scales. Journal of the American Chemical Society, 2005, 127(37): 13055–13059

    Article  CAS  Google Scholar 

  35. Adrian B. Constructal-theory network of conducting paths for cooling a heat generating volume. International Journal of Heat and Mass Transfer, 1997, 40(4): 799–816

    Article  Google Scholar 

  36. Gheorghiu S, Coppens M O. Optimal bimodal pore networks for heterogeneous catalysis. AIChE Journal. American Institute of Chemical Engineers, 2004, 50(4): 812–820

    Article  CAS  Google Scholar 

  37. Wang X, Yu J C, Ho C, Hou Y, Fu X. Photocatalytic activity of a hierarchically macro/mesoporous titania. Langmuir, 2005, 21(6): 2552–2559

    Article  CAS  Google Scholar 

  38. Dong F, Lee S C, Wu Z, Huang Y, Fu M, Ho W K, Zou S, Wang B. Rose-like monodisperse bismuth subcarbonate hierarchical hollow microspheres: one-pot template-free fabrication and excellent visible light photocatalytic activity and photochemical stability for NO removal in indoor air. Journal of Hazardous Materials, 2011, 195: 346–354

    Article  CAS  Google Scholar 

  39. Dong F, Sun Y, Ho W K, Wu Z. Controlled synthesis, growth mechanism and highly efficient solar photocatalysis of nitrogendoped bismuth subcarbonate hierarchical nanosheets architectures. Dalton Transactions (Cambridge, England), 2012, 41(27): 8270–8284

    Article  CAS  Google Scholar 

  40. Parlett C M A, Wilson K, Lee A F. Hierarchical porous materials: catalytic applications. Chemical Society Reviews, 2013, 42(9): 3876–3893

    Article  CAS  Google Scholar 

  41. Liu G, Yang K, Li J Q, Tang W X, Xu J B, Liu H D, Yue R L, Chen Y F. Surface diffusion of Pt clusters in/on SiO2 matrix at elevated temperatures and their improved catalytic activities in benzene oxidation. Journal of Physical Chemistry C, 2014, 118(39): 22719–22729

    Article  CAS  Google Scholar 

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Correspondence to Zhengping Hao.

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Qiao, N., Zhang, X., He, C. et al. Enhanced performances in catalytic oxidation of o-xylene over hierarchical macro-/mesoporous silica-supported palladium catalysts. Front. Environ. Sci. Eng. 10, 458–466 (2016). https://doi.org/10.1007/s11783-015-0802-1

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