Final Report: Development of Nanocrystalline Zeolite Materials as Environmental Catalysts: From Environmentally Benign Synthesis to Emission Abatement

EPA Grant Number: R829600
Title: Development of Nanocrystalline Zeolite Materials as Environmental Catalysts: From Environmentally Benign Synthesis to Emission Abatement
Investigators: Larsen, Sarah C. , Grassian, Vicki H.
Institution: University of Iowa
EPA Project Officer: Lasat, Mitch
Project Period: January 1, 2002 through December 31, 2004
Project Amount: $350,000
RFA: Exploratory Research: Nanotechnology (2001) RFA Text |  Recipients Lists
Research Category: Nanotechnology , Safer Chemicals

Objective:

The goal of this research project was to develop nanometer-sized zeolites and zeolite nanostructures as environmental catalysts. Zeolites, which are widely used in applications in separations and catalysis, are aluminosilicate molecular sieves with pores of molecular dimensions. The crystal size of zeolites formed during conventional synthesis range in size from 1,000 to 10,000 nm. For some applications, however, it would be advantageous to employ much smaller nanometer-sized zeolite crystals in the range of 10-100 nm. Specific advantages to be gained by using zeolite nanostructures include facile adsorption and desorption, the ability to form dense films to facilitate separations applications, and optical transparency. The specific objectives of this research project were to: (1) synthesis and characterize nanocrystalline zeolites; and (2) use the nanocrystalline zeolites as environmental catalysts.

Summary/Accomplishments (Outputs/Outcomes):

The major accomplishments during Year 3 of the project are:

  • Synthesis of nanocrystalline silicalite-1, NaZSM-5, and NaY with particle sizes of 15-20 nm and external surface areas greater than 100 m2/g.
  • Characterization of the silicalite-1, NaZSM-5, and NaY by powder X-ray diffraction, scanning electron microscopy, nitrogen adsorption isotherms, and solid state nuclear magnetic resonance.
  • Study of the adsorption and desorption of a representative volatile organic compound, such as toluene, on silicalite-1, NaZSM-5, and NaY.
  • Development of a more efficient synthesis method for nanocrystalline silicalite and NaY involving the recycling of the synthesis solution.
  • Investigation of the self-assembly of silicalite-1 nanocrystals into rectangular fibers.
  • Functionalization of the external surface of nanocrystalline ZSM-5and NaY to increase hydrophobicity.
  • Preparation of hollow zeolite structures using nanocrystalline silicalite as a building block.
  • Incorporation of aluminum into the hollow zeolite structures.
  • Usage of Fourier Transform Infrared Spectroscopy to investigate the use of nanocrystalline NaY for the selective catalytic reduction of NOx with propylene and urea.
  • Demonstration that nanocrystalline NaY is a superior catalyst for urea selective catalytic reduction relative to Aldrich NaY.


Journal Articles on this Report : 11 Displayed | Download in RIS Format

Other project views: All 47 publications 16 publications in selected types All 11 journal articles
Type Citation Project Document Sources
Journal Article Li GH, Larsen SC, Grassian VH. Catalytic reduction of NO2 in nanocrystalline NaY zeolite. Journal of Molecular Catalysis A-Chemical 2005;227(1-2):25-35. R829600 (2004)
R829600 (Final)
not available
Journal Article Li GH, Jones CA, Grassian VH, Larsen SC. Selective catalytic reduction of NO2 with urea in nanocrystalline NaY zeolite. Journal of Catalysis 2005;234(2):401-413. R829600 (Final)
not available
Journal Article Li G, Xu M, Larsen SC, Grassian VH. Photooxidation of cyclohexane and cyclohexene in bay. Journal of Molecular Catalysis A: Chemical 2003;194(1-2):169-180. R829600 (2002)
R829600 (Final)
not available
Journal Article Li GH, Larsen SC, Grassian VH. An FT-IR study of NO2 reduction in nanocrystalline NaY zeolite: effect of zeolite crystal size and adsorbed water. Catalysis Letters 2005;103(1-2):23-32 R829600 (2004)
R829600 (Final)
not available
Journal Article Song W, Kanthasamy R, Grassian VH, Larsen SC. Hexagonal, hollow, aluminium-containing ZSM-5 tubes prepared from mesoporous silica templates. Chemical Communications 2004;(17):1920-1921 R829600 (2004)
R829600 (Final)
not available
Journal Article Song W, Justice RE, Jones CA, Grassian VH. Size-dependent properties of nanocrystalline silicalite synthesized with systematically varied crystal sizes. Langmuir 2004;20(11):4696-4702. R829600 (2004)
R829600 (Final)
not available
Journal Article Song W, Justice RE, Jones CA, Grassian VH, Larsen SC. Synthesis, characterization, and adsorption properties of nanocrystalline ZSM-5. Langmuir 2004;20(19):8301-8306 R829600 (2004)
R829600 (Final)
not available
Journal Article Song W, Li G, Grassian VH, Larsen SC. Development of improved materials for environmental applications: Nanocrystalline NaY zeolites. Environmental Science & Technology 2005;39(5):1214-1220. R829600 (2004)
R829600 (Final)
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  • Journal Article Song W, Grassian VH, Larsen SC. High yield method for nanocrystalline zeolite synthesis. Chemical Communications 2005;(23):2951-2953. R829600 (2004)
    R829600 (Final)
    not available
    Journal Article Song W, Woodworth JF, Grassian VH, Larsen SC. Microscopic and macroscopic characterization of organosilane-functionalized nanocrystalline NaZSM-5. Langmuir 2005;21(15):7009-7014. R829600 (2004)
    R829600 (Final)
    not available
    Journal Article Song W, Grassian VH, Larsen SC. Fiber and film formation by self-assembly of colloidal silicalite-1 and copper coated silicalite-1 nanocrystals. Microporous and Mesoporous Materials 2006;88(1-3):77-83. R829600 (Final)
    not available

    Supplemental Keywords:

    Supplemental Keywords: pollution prevention, clean technologies, pollution prevention, green chemistry, nanotechnology, waste minimization, remediation, VOC, nitrogen oxides, solvents, oxidation,, Scientific Discipline, Toxics, Waste, Sustainable Industry/Business, Chemical Engineering, cleaner production/pollution prevention, Remediation, Environmental Chemistry, HAPS, VOCs, Chemistry and Materials Science, Environmental Engineering, environmentally benign synthesis, Nox, Nitrogen Oxides, waste minimization, zeolites, clean technology, nanotechnology, nitrogen oxide, environmental catalysts, nanomaterials, pollution prevention, nanocrystalline zeolite materials, emission abatement, green chemistry

    Relevant Websites:

    http://www.chem.uiowa.edu/faculty/larsen/index.html Exit
    http://www.chem.uiowa.edu/faculty/grassian/index.html Exit

    Progress and Final Reports:

    Original Abstract
  • 2002 Progress Report
  • 2003