Gel-based morphological design of zirconium metal–organic frameworks

The ability of metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the f...

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Vydané v:	Chemical science (Cambridge) Ročník 8; číslo 5; s. 3939 - 3948
Hlavní autori:	Bueken, Bart, Van Velthoven, Niels, Willhammar, Tom, Stassin, Timothée, Stassen, Ivo, Keen, David A., Baron, Gino V., Denayer, Joeri F. M., Ameloot, Rob, Bals, Sara, De Vos, Dirk, Bennett, Thomas D.
Médium:	Journal Article
Jazyk:	English
Vydavateľské údaje:	England Royal Society of Chemistry 01.05.2017
Predmet:	Adsorptivity Catalysis Catalysts Chemistry Gels Mass transfer Metal-organic frameworks Nanoparticles Porosity
ISSN:	2041-6520, 2041-6539, 2041-6539
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Abstract	The ability of metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr 4+ -based MOFs: UiO-66-X (X = H, NH 2 , NO 2 , (OH) 2 ), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO 2 . Electron microscopy, combined with N 2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 μm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations.
AbstractList	The ability of metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr 4+ -based MOFs: UiO-66-X (X = H, NH 2 , NO 2 , (OH) 2 ), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO 2 . Electron microscopy, combined with N 2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 μm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X = H, NH2, NO2, (OH)2), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 μm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations.The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X = H, NH2, NO2, (OH)2), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 μm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X = H, NH2, NO2, (OH)2), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mu m diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr -based MOFs: UiO-66-X (X = H, NH , NO , (OH) ), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO . Electron microscopy, combined with N physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 μm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero-or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X - H, NH2, NO2, (OH)(2)), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N-2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations. The ability of zirconium metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. The ability of metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero- or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X = H, NH2, NO2, (OH)2), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 μm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations.
Author	De Vos, Dirk Keen, David A. Willhammar, Tom Bueken, Bart Baron, Gino V. Ameloot, Rob Van Velthoven, Niels Stassen, Ivo Denayer, Joeri F. M. Stassin, Timothée Bals, Sara Bennett, Thomas D.
AuthorAffiliation	e Department of Chemical Engineering , Vrije Universiteit Brussel , Pleinlaan 2 , 1050 Brussels , Belgium c Department of Materials and Environmental Chemistry , Stockholm University , S-106 91 Stockholm , Sweden a Centre for Surface Chemistry and Catalysis , Department of Microbial and Molecular Systems (M2S) , KU Leuven , Celestijnenlaan 200F p.o. box 2461 , 3001 Leuven , Belgium . Email: dirk.devos@kuleuven.be d ISIS Facility , Rutherford Appleton Laboratory , Harwell Campus , Didcot , Oxon OX11 0QX , UK f Department of Materials Science and Metallurgy , University of Cambridge , 27 Charles Babbage Road , Cambridge CB3 0FS , UK . Email: tdb35@cam.ac.uk b EMAT , University of Antwerp , Groenenborgerlaan 171 , 2020 Antwerp , Belgium
AuthorAffiliation_xml	– name: c Department of Materials and Environmental Chemistry , Stockholm University , S-106 91 Stockholm , Sweden – name: f Department of Materials Science and Metallurgy , University of Cambridge , 27 Charles Babbage Road , Cambridge CB3 0FS , UK . Email: tdb35@cam.ac.uk – name: b EMAT , University of Antwerp , Groenenborgerlaan 171 , 2020 Antwerp , Belgium – name: e Department of Chemical Engineering , Vrije Universiteit Brussel , Pleinlaan 2 , 1050 Brussels , Belgium – name: a Centre for Surface Chemistry and Catalysis , Department of Microbial and Molecular Systems (M2S) , KU Leuven , Celestijnenlaan 200F p.o. box 2461 , 3001 Leuven , Belgium . Email: dirk.devos@kuleuven.be – name: d ISIS Facility , Rutherford Appleton Laboratory , Harwell Campus , Didcot , Oxon OX11 0QX , UK
Author_xml	– sequence: 1 givenname: Bart orcidid: 0000-0002-4610-7204 surname: Bueken fullname: Bueken, Bart organization: Centre for Surface Chemistry and Catalysis, Department of Microbial and Molecular Systems (M2S), KU Leuven, 3001 Leuven, Belgium – sequence: 2 givenname: Niels surname: Van Velthoven fullname: Van Velthoven, Niels organization: Centre for Surface Chemistry and Catalysis, Department of Microbial and Molecular Systems (M2S), KU Leuven, 3001 Leuven, Belgium – sequence: 3 givenname: Tom orcidid: 0000-0001-6120-1218 surname: Willhammar fullname: Willhammar, Tom organization: EMAT, University of Antwerp, 2020 Antwerp, Belgium, Department of Materials and Environmental Chemistry – sequence: 4 givenname: Timothée surname: Stassin fullname: Stassin, Timothée organization: Centre for Surface Chemistry and Catalysis, Department of Microbial and Molecular Systems (M2S), KU Leuven, 3001 Leuven, Belgium – sequence: 5 givenname: Ivo orcidid: 0000-0003-3997-653X surname: Stassen fullname: Stassen, Ivo organization: Centre for Surface Chemistry and Catalysis, Department of Microbial and Molecular Systems (M2S), KU Leuven, 3001 Leuven, Belgium – sequence: 6 givenname: David A. surname: Keen fullname: Keen, David A. organization: ISIS Facility, Rutherford Appleton Laboratory, Didcot, UK – sequence: 7 givenname: Gino V. surname: Baron fullname: Baron, Gino V. organization: Department of Chemical Engineering, Vrije Universiteit Brussel, 1050 Brussels, Belgium – sequence: 8 givenname: Joeri F. M. surname: Denayer fullname: Denayer, Joeri F. M. organization: Department of Chemical Engineering, Vrije Universiteit Brussel, 1050 Brussels, Belgium – sequence: 9 givenname: Rob orcidid: 0000-0003-3178-5480 surname: Ameloot fullname: Ameloot, Rob organization: Centre for Surface Chemistry and Catalysis, Department of Microbial and Molecular Systems (M2S), KU Leuven, 3001 Leuven, Belgium – sequence: 10 givenname: Sara surname: Bals fullname: Bals, Sara organization: EMAT, University of Antwerp, 2020 Antwerp, Belgium – sequence: 11 givenname: Dirk surname: De Vos fullname: De Vos, Dirk organization: Centre for Surface Chemistry and Catalysis, Department of Microbial and Molecular Systems (M2S), KU Leuven, 3001 Leuven, Belgium – sequence: 12 givenname: Thomas D. orcidid: 0000-0003-3717-3119 surname: Bennett fullname: Bennett, Thomas D. organization: Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/28553536$$D View this record in MEDLINE/PubMed https://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-143393$$DView record from Swedish Publication Index (Stockholms universitet)
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Snippet	The ability of metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of... The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of... The ability of zirconium metal–organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and...
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SubjectTerms	Adsorptivity Catalysis Catalysts Chemistry Gels Mass transfer Metal-organic frameworks Nanoparticles Porosity
Title	Gel-based morphological design of zirconium metal–organic frameworks
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