Ethylene Epoxidation Catalyzed by Ag Nanoparticles on Ag-LSX Zeolites formed by Pressure- and Temperature-Induced Auto-Reduction

Donghoon Kim, Yongmoon Lee, Yonghwi Kim, Kathleen Mingle, Jochen Lauterbach, Douglas A. Blom, Thomas Vogt, Yongjae Lee

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

Ag+-Exchanged LSX (Ag-LSX: Ag96Al96Si96O384⋅n H2O), a large pore low silica analogue (Si/Al=1.0) of faujasite, was prepared and post-synthetically modified using pressure and temperature in the presence of various pore-penetrating fluids. Using high-resolution synchrotron X-ray powder and single crystal diffraction we derive structural models of the as-prepared and post-synthetically modified Ag-LSX materials. In the as-prepared Ag-LSX model, we located 96 silver cations and 245 H2O molecules distributed over seven and five distinctive sites, respectively. At 1.4(1) GPa pressure and 150 °C in ethanol the number of silver cations within the pores of Ag-LSX is reduced by ca. 47.4 %, whereas the number of H2O molecules is increased by ca. 40.8 %. The formation of zero-valent silver nanoparticles deposited on Ag-LSX crystallites depends on the fluid present during pressurization. Ag-nanoparticle-Ag-zeolite hybrid materials are recovered after pressure release and shown to have different chemical reactivity when used as catalysts for ethylene epoxidation.

Original languageEnglish
Pages (from-to)1041-1045
Number of pages5
JournalChemistry - A European Journal
Volume24
Issue number5
DOIs
Publication statusPublished - 2018 Jan 24

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Zeolites
Epoxidation
Silver
Ethylene
Nanoparticles
Cations
Positive ions
Chemical reactivity
Molecules
Fluids
Pressurization
Hybrid materials
Synchrotrons
Crystallites
Silicon Dioxide
Powders
Temperature
Ethanol
Diffraction
Silica

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Organic Chemistry

Cite this

Kim, Donghoon ; Lee, Yongmoon ; Kim, Yonghwi ; Mingle, Kathleen ; Lauterbach, Jochen ; Blom, Douglas A. ; Vogt, Thomas ; Lee, Yongjae. / Ethylene Epoxidation Catalyzed by Ag Nanoparticles on Ag-LSX Zeolites formed by Pressure- and Temperature-Induced Auto-Reduction. In: Chemistry - A European Journal. 2018 ; Vol. 24, No. 5. pp. 1041-1045.
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Ethylene Epoxidation Catalyzed by Ag Nanoparticles on Ag-LSX Zeolites formed by Pressure- and Temperature-Induced Auto-Reduction. / Kim, Donghoon; Lee, Yongmoon; Kim, Yonghwi; Mingle, Kathleen; Lauterbach, Jochen; Blom, Douglas A.; Vogt, Thomas; Lee, Yongjae.

In: Chemistry - A European Journal, Vol. 24, No. 5, 24.01.2018, p. 1041-1045.

Research output: Contribution to journalArticle

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T1 - Ethylene Epoxidation Catalyzed by Ag Nanoparticles on Ag-LSX Zeolites formed by Pressure- and Temperature-Induced Auto-Reduction

AU - Kim, Donghoon

AU - Lee, Yongmoon

AU - Kim, Yonghwi

AU - Mingle, Kathleen

AU - Lauterbach, Jochen

AU - Blom, Douglas A.

AU - Vogt, Thomas

AU - Lee, Yongjae

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N2 - Ag+-Exchanged LSX (Ag-LSX: Ag96Al96Si96O384⋅n H2O), a large pore low silica analogue (Si/Al=1.0) of faujasite, was prepared and post-synthetically modified using pressure and temperature in the presence of various pore-penetrating fluids. Using high-resolution synchrotron X-ray powder and single crystal diffraction we derive structural models of the as-prepared and post-synthetically modified Ag-LSX materials. In the as-prepared Ag-LSX model, we located 96 silver cations and 245 H2O molecules distributed over seven and five distinctive sites, respectively. At 1.4(1) GPa pressure and 150 °C in ethanol the number of silver cations within the pores of Ag-LSX is reduced by ca. 47.4 %, whereas the number of H2O molecules is increased by ca. 40.8 %. The formation of zero-valent silver nanoparticles deposited on Ag-LSX crystallites depends on the fluid present during pressurization. Ag-nanoparticle-Ag-zeolite hybrid materials are recovered after pressure release and shown to have different chemical reactivity when used as catalysts for ethylene epoxidation.

AB - Ag+-Exchanged LSX (Ag-LSX: Ag96Al96Si96O384⋅n H2O), a large pore low silica analogue (Si/Al=1.0) of faujasite, was prepared and post-synthetically modified using pressure and temperature in the presence of various pore-penetrating fluids. Using high-resolution synchrotron X-ray powder and single crystal diffraction we derive structural models of the as-prepared and post-synthetically modified Ag-LSX materials. In the as-prepared Ag-LSX model, we located 96 silver cations and 245 H2O molecules distributed over seven and five distinctive sites, respectively. At 1.4(1) GPa pressure and 150 °C in ethanol the number of silver cations within the pores of Ag-LSX is reduced by ca. 47.4 %, whereas the number of H2O molecules is increased by ca. 40.8 %. The formation of zero-valent silver nanoparticles deposited on Ag-LSX crystallites depends on the fluid present during pressurization. Ag-nanoparticle-Ag-zeolite hybrid materials are recovered after pressure release and shown to have different chemical reactivity when used as catalysts for ethylene epoxidation.

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