Assessing Inter and Intra-particle Heterogeneity in Alumina-poor H-ZSM-5 Zeolites

被引:12
作者
Kennes, Koen [1 ]
Demaret, Coralie [2 ]
Van Loon, Jordi [1 ]
Kubarev, Alexey V. [1 ]
Fleury, Guillaume [1 ]
Sliwa, Michel [3 ]
Delpoux, Olivier [2 ]
Maury, Sylvie [2 ]
Harbuzaru, Bogdan [2 ]
Roeffaers, Maarten B. J. [1 ]
机构
[1] Katholieke Univ Leuven, Fac Biosci Engn, Ctr Surface Chem & Catalysis, Kasteelpk Arenberg 23, B-3001 Heverlee, Belgium
[2] IFP Energies Nouvelles, Lyon Estab, Rond Point Echangeur Solaize BP 3, F-69360 Solaize, France
[3] Univ Lille, CNRS, UMR 8516, Lab Spectrochim Infrarouge & Raman LASI, F-59000 Lille, France
基金
欧洲研究理事会;
关键词
acidity; electron microscopy; macropores; mesopores; super-resolution fluorescence microscopy; zeolites; METAL-ORGANIC FRAMEWORK; SI/AL RATIO; FLUORESCENCE MICROSCOPY; AMMONIUM EXCHANGE; ZSM-5; CRYSTALS; ACTIVE-SITES; SINGLE; REACTIVITY; MORPHOLOGY; PARTICLES;
D O I
10.1002/cctc.201700696
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
We reveal the presence of significant variations in Bronsted catalytic activity within and between individual H-ZSM-5 zeolite crystals. Fluorescence microscopy in combination with a fluorogenic probe was used to resolve the catalytic activity at the nanoscale. The observed variations in catalytic activity could be directly linked to structural parameters and crystal morphology observed in scanning electron microscopy and by specifically staining crystal defects. The obtained results are directly compared with ensemble averaged information from techniques such as pyridine IR spectroscopy and nitrogen physisorption, typically used to characterize acid zeolites. The inter- and intra-particle heterogeneities resolved by the employed fluorescence approach remain unaddressed by bulk characterization. Our experimental results relate the heterogeneous catalytic activity to variation in both the Si/Al ratio and mesoporosity induced during the zeolite synthesis.
引用
收藏
页码:3440 / 3445
页数:6
相关论文
共 36 条
  • [1] Synthesis and applications of metal-organic framework-quantum dot (QD@MOF) composites
    Aguilera-Sigalat, Jordi
    Bradshaw, Darren
    [J]. COORDINATION CHEMISTRY REVIEWS, 2016, 307 : 267 - 291
  • [2] [Anonymous], 2015, ANGEW CHEM, V127, P1856
  • [3] [Anonymous], 2009, ANGEW CHEM, V121, P9449
  • [4] Functionalized gold nanoclusters as fluorescent labels for immunoassays: Application to human serum immunoglobulin E determination
    Cruz Alonso, Maria
    Trapiella-Alfonso, Laura
    Costa Fernandez, Jose M.
    Pereiro, Rosario
    Sanz-Medel, Alfredo
    [J]. BIOSENSORS & BIOELECTRONICS, 2016, 77 : 1055 - 1061
  • [5] Where Are the Active Sites in Zeolites? Origin of Aluminum Zoning in ZSM-5
    Danilina, Nadiya
    Krumeich, Frank
    Castelanelli, Stefano A.
    van Bokhoven, Jeroen A.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (14) : 6640 - 6645
  • [6] Differences Between Individual ZSM-5 Crystals in Forming Hollow Single Crystals and Mesopores During Base Leaching
    Fodor, Daniel
    Krumeich, Frank
    Hauert, Roland
    van Bokhoven, Jeroen A.
    [J]. CHEMISTRY-A EUROPEAN JOURNAL, 2015, 21 (16) : 6272 - 6277
  • [7] Determination of Si/Al molar ratios in microporous zeolites using calibration-free laser induced breakdown spectroscopy
    Hornackova, M.
    Hornacek, M.
    Rakovsky, J.
    Hudec, P.
    Veis, P.
    [J]. SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY, 2013, 88 : 69 - 74
  • [8] Centimeter-sized zeolite bodies of intergrown crystals: Preparation, characterization and study of binder evolution
    Itani, Lama
    Valtchev, Valentin
    Patarin, Joel
    Rigolet, Severinne
    Gao, Feifei
    Baudin, Gerard
    [J]. MICROPOROUS AND MESOPOROUS MATERIALS, 2011, 138 (1-3) : 157 - 166
  • [9] Single molecule methods for the study of catalysis: from enzymes to heterogeneous catalysts
    Janssen, Kris P. F.
    De Cremer, Gert
    Neely, Robert K.
    Kubarev, Alexey V.
    Van Loon, Jordi
    Martens, Johan A.
    De Vos, Dirk E.
    Roeffaers, Maarten B. J.
    Hofkens, Johan
    [J]. CHEMICAL SOCIETY REVIEWS, 2014, 43 (04) : 990 - 1006
  • [10] Low-temperature CO oxidation on Ag/ZSM-5 catalysts: Influence of Si/Al ratio and redox pretreatments on formation of silver active sites
    Kolobova, E.
    Pestryakov, A.
    Mamontov, G.
    Kotolevich, Yu.
    Bogdanchikova, N.
    Farias, M.
    Vosmerikov, A.
    Vosmerikova, L.
    Cortes Corberan, V.
    [J]. FUEL, 2017, 188 : 121 - 131