Metal-organic frameworks as catalyst supports : influence of defects on metal nanoparticle formation

Miguel Rivera-Torrente, Matthias Filez, Rifan Hardian, Emily Reynolds, Beatriz Seoane, Marie Vanessa Coulet, Freddy E. Oropeza Palacio, Jan P. Hofmann, Roland A. Fischer, Andrew L. Goodwin, Philip L. Llewellyn, Bert M. Weckhuysen

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Abstract

Because of their high tunability and surface area, metal-organic frameworks (MOFs) show great promise as supports for metal nanoparticles. Depending on the synthesis route, MOFs may contain defects. Here, we show that highly crystalline MIL-100(Fe) and disordered Basolite® F300, with identical iron 1,3,5-benzenetricarboxylate composition, exhibit very divergent properties when used as a support for Pd nanoparticle deposition. While MIL-100(Fe) shows a regular MTN-zeotype crystal structure with two types of cages, Basolite® F300 lacks long-range order beyond 8Å and has a single-pore system. The medium-range configurational linker-node disorder in Basolite® F300 results in a reduced number of Lewis acid sites, yielding more hydrophobic surface properties compared to hydrophilic MIL-100(Fe). The hydrophilic/hydrophobic nature of MIL-100(Fe) and Basolite® F300 impacts the amount of Pd and particle size distribution of Pd nanoparticles deposited during colloidal synthesis and dry impregnation methods, respectively. It is suggested that polar (apolar) solvents/precursors attractively interact with hydrophilic (hydrophobic) MOF surfaces, allowing tools at hand to increase the level of control over, for example, the nanoparticle size distribution.

Original languageEnglish
JournalChemistry : A European Journal
Volume24
Issue number29
DOIs
Publication statusPublished - 30 Apr 2018

Fingerprint

Metal nanoparticles
Catalyst supports
Metals
Nanoparticles
Defects
Impregnation
Particle size analysis
Lewis Acids
Surface properties
Crystal structure
Iron
Crystalline materials
Acids
Chemical analysis
N(1)-methyl-2-lysergic acid diethylamide

Keywords

  • Basolite
  • Heterogeneous catalysis
  • Lattice disorder
  • Metal-organic frameworks (MOF)
  • MIL-100 (Fe)
  • Pd nanoparticles

Cite this

Rivera-Torrente, M., Filez, M., Hardian, R., Reynolds, E., Seoane, B., Coulet, M. V., ... Weckhuysen, B. M. (2018). Metal-organic frameworks as catalyst supports : influence of defects on metal nanoparticle formation. Chemistry : A European Journal, 24(29). https://doi.org/10.1002/chem.201800694
Rivera-Torrente, Miguel ; Filez, Matthias ; Hardian, Rifan ; Reynolds, Emily ; Seoane, Beatriz ; Coulet, Marie Vanessa ; Oropeza Palacio, Freddy E. ; Hofmann, Jan P. ; Fischer, Roland A. ; Goodwin, Andrew L. ; Llewellyn, Philip L. ; Weckhuysen, Bert M. / Metal-organic frameworks as catalyst supports : influence of defects on metal nanoparticle formation. In: Chemistry : A European Journal. 2018 ; Vol. 24, No. 29.
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abstract = "Because of their high tunability and surface area, metal-organic frameworks (MOFs) show great promise as supports for metal nanoparticles. Depending on the synthesis route, MOFs may contain defects. Here, we show that highly crystalline MIL-100(Fe) and disordered Basolite{\circledR} F300, with identical iron 1,3,5-benzenetricarboxylate composition, exhibit very divergent properties when used as a support for Pd nanoparticle deposition. While MIL-100(Fe) shows a regular MTN-zeotype crystal structure with two types of cages, Basolite{\circledR} F300 lacks long-range order beyond 8{\AA} and has a single-pore system. The medium-range configurational linker-node disorder in Basolite{\circledR} F300 results in a reduced number of Lewis acid sites, yielding more hydrophobic surface properties compared to hydrophilic MIL-100(Fe). The hydrophilic/hydrophobic nature of MIL-100(Fe) and Basolite{\circledR} F300 impacts the amount of Pd and particle size distribution of Pd nanoparticles deposited during colloidal synthesis and dry impregnation methods, respectively. It is suggested that polar (apolar) solvents/precursors attractively interact with hydrophilic (hydrophobic) MOF surfaces, allowing tools at hand to increase the level of control over, for example, the nanoparticle size distribution.",
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author = "Miguel Rivera-Torrente and Matthias Filez and Rifan Hardian and Emily Reynolds and Beatriz Seoane and Coulet, {Marie Vanessa} and {Oropeza Palacio}, {Freddy E.} and Hofmann, {Jan P.} and Fischer, {Roland A.} and Goodwin, {Andrew L.} and Llewellyn, {Philip L.} and Weckhuysen, {Bert M.}",
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Rivera-Torrente, M, Filez, M, Hardian, R, Reynolds, E, Seoane, B, Coulet, MV, Oropeza Palacio, FE, Hofmann, JP, Fischer, RA, Goodwin, AL, Llewellyn, PL & Weckhuysen, BM 2018, 'Metal-organic frameworks as catalyst supports : influence of defects on metal nanoparticle formation', Chemistry : A European Journal, vol. 24, no. 29. https://doi.org/10.1002/chem.201800694

Metal-organic frameworks as catalyst supports : influence of defects on metal nanoparticle formation. / Rivera-Torrente, Miguel; Filez, Matthias; Hardian, Rifan; Reynolds, Emily; Seoane, Beatriz; Coulet, Marie Vanessa; Oropeza Palacio, Freddy E.; Hofmann, Jan P.; Fischer, Roland A.; Goodwin, Andrew L.; Llewellyn, Philip L.; Weckhuysen, Bert M.

In: Chemistry : A European Journal, Vol. 24, No. 29, 30.04.2018.

Research output: Contribution to journalArticleAcademicpeer-review

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T1 - Metal-organic frameworks as catalyst supports : influence of defects on metal nanoparticle formation

AU - Rivera-Torrente, Miguel

AU - Filez, Matthias

AU - Hardian, Rifan

AU - Reynolds, Emily

AU - Seoane, Beatriz

AU - Coulet, Marie Vanessa

AU - Oropeza Palacio, Freddy E.

AU - Hofmann, Jan P.

AU - Fischer, Roland A.

AU - Goodwin, Andrew L.

AU - Llewellyn, Philip L.

AU - Weckhuysen, Bert M.

PY - 2018/4/30

Y1 - 2018/4/30

N2 - Because of their high tunability and surface area, metal-organic frameworks (MOFs) show great promise as supports for metal nanoparticles. Depending on the synthesis route, MOFs may contain defects. Here, we show that highly crystalline MIL-100(Fe) and disordered Basolite® F300, with identical iron 1,3,5-benzenetricarboxylate composition, exhibit very divergent properties when used as a support for Pd nanoparticle deposition. While MIL-100(Fe) shows a regular MTN-zeotype crystal structure with two types of cages, Basolite® F300 lacks long-range order beyond 8Å and has a single-pore system. The medium-range configurational linker-node disorder in Basolite® F300 results in a reduced number of Lewis acid sites, yielding more hydrophobic surface properties compared to hydrophilic MIL-100(Fe). The hydrophilic/hydrophobic nature of MIL-100(Fe) and Basolite® F300 impacts the amount of Pd and particle size distribution of Pd nanoparticles deposited during colloidal synthesis and dry impregnation methods, respectively. It is suggested that polar (apolar) solvents/precursors attractively interact with hydrophilic (hydrophobic) MOF surfaces, allowing tools at hand to increase the level of control over, for example, the nanoparticle size distribution.

AB - Because of their high tunability and surface area, metal-organic frameworks (MOFs) show great promise as supports for metal nanoparticles. Depending on the synthesis route, MOFs may contain defects. Here, we show that highly crystalline MIL-100(Fe) and disordered Basolite® F300, with identical iron 1,3,5-benzenetricarboxylate composition, exhibit very divergent properties when used as a support for Pd nanoparticle deposition. While MIL-100(Fe) shows a regular MTN-zeotype crystal structure with two types of cages, Basolite® F300 lacks long-range order beyond 8Å and has a single-pore system. The medium-range configurational linker-node disorder in Basolite® F300 results in a reduced number of Lewis acid sites, yielding more hydrophobic surface properties compared to hydrophilic MIL-100(Fe). The hydrophilic/hydrophobic nature of MIL-100(Fe) and Basolite® F300 impacts the amount of Pd and particle size distribution of Pd nanoparticles deposited during colloidal synthesis and dry impregnation methods, respectively. It is suggested that polar (apolar) solvents/precursors attractively interact with hydrophilic (hydrophobic) MOF surfaces, allowing tools at hand to increase the level of control over, for example, the nanoparticle size distribution.

KW - Basolite

KW - Heterogeneous catalysis

KW - Lattice disorder

KW - Metal-organic frameworks (MOF)

KW - MIL-100 (Fe)

KW - Pd nanoparticles

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DO - 10.1002/chem.201800694

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