Metal-Organic Frameworks: Building Block Design Strategies for the Synthesis of MOFs.

Handle URI:
http://hdl.handle.net/10754/336368
Title:
Metal-Organic Frameworks: Building Block Design Strategies for the Synthesis of MOFs.
Authors:
Luebke, Ryan ( 0000-0002-1285-3321 )
Abstract:
A significant and ongoing challenge in materials chemistry and furthermore solid state chemistry is to design materials with the desired properties and characteristics. The field of Metal-Organic Frameworks (MOFs) offers several strategies to address this challenge and has proven fruitful at allowing some degree of control over the resultant materials synthesized. Several methodologies for synthesis of MOFs have been developed which rely on use of predetermined building blocks. The work presented herein is focused on the utilization of two of these design principles, namely the use of molecular building blocks (MBBs) and supermolecular building blocks (SBBs) to target MOF materials having desired connectivities (topologies). These design strategies also permit the introduction of specific chemical moieties, allowing for modification of the MOFs properties. This research is predominantly focused on two platforms (rht-MOFs and ftw-MOFs) which topologically speaking are edge transitive binodal nets; ftw being a (4,12)-connected net and rht being a (3,24)-connected net. These highly connected nets (at least one node having connectivity greater than eight) have been purposefully targeted to increase the predictability of structural outcome. A general trend in topology is that there is an inverse relationship between the connectivity of the node(s) and the number of topological outcomes. Therefore the key to this research (and to effective use of the SBB and MBB approaches) is identification of conditions which allow for reliable formation of the targeted MBBs and SBBs. In the case of the research presented herein: a 12-connected Group IV or Rare Earth based hexanuclear MBB and a 24-connected transition metal based SBB were successfully targeted and synthesized. These two synthetic platforms will be presented and used as examples of how these design methods have been (and can be further) utilized to modify existing materials or develop new materials for gas storage and separation applications for environmental and energy related applications including hydrogen, methane, carbon dioxide and hydrocarbon storage or separations.
Advisors:
Eddaoudi, Mohamed ( 0000-0003-1916-9837 )
Committee Member:
Pinnau, Ingo ( 0000-0003-3040-9088 ) ; Takanabe, Kazuhiro ( 0000-0001-5374-9451 ) ; Zaworotko, Michael
KAUST Department:
Physical Sciences and Engineering (PSE) Division
Program:
Chemical Sciences
Issue Date:
Sep-2014
Type:
Dissertation
Appears in Collections:
Dissertations; Physical Sciences and Engineering (PSE) Division; Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.advisorEddaoudi, Mohameden
dc.contributor.authorLuebke, Ryanen
dc.date.accessioned2014-11-30T10:59:31Z-
dc.date.available2014-11-30T10:59:31Z-
dc.date.issued2014-09en
dc.identifier.urihttp://hdl.handle.net/10754/336368en
dc.description.abstractA significant and ongoing challenge in materials chemistry and furthermore solid state chemistry is to design materials with the desired properties and characteristics. The field of Metal-Organic Frameworks (MOFs) offers several strategies to address this challenge and has proven fruitful at allowing some degree of control over the resultant materials synthesized. Several methodologies for synthesis of MOFs have been developed which rely on use of predetermined building blocks. The work presented herein is focused on the utilization of two of these design principles, namely the use of molecular building blocks (MBBs) and supermolecular building blocks (SBBs) to target MOF materials having desired connectivities (topologies). These design strategies also permit the introduction of specific chemical moieties, allowing for modification of the MOFs properties. This research is predominantly focused on two platforms (rht-MOFs and ftw-MOFs) which topologically speaking are edge transitive binodal nets; ftw being a (4,12)-connected net and rht being a (3,24)-connected net. These highly connected nets (at least one node having connectivity greater than eight) have been purposefully targeted to increase the predictability of structural outcome. A general trend in topology is that there is an inverse relationship between the connectivity of the node(s) and the number of topological outcomes. Therefore the key to this research (and to effective use of the SBB and MBB approaches) is identification of conditions which allow for reliable formation of the targeted MBBs and SBBs. In the case of the research presented herein: a 12-connected Group IV or Rare Earth based hexanuclear MBB and a 24-connected transition metal based SBB were successfully targeted and synthesized. These two synthetic platforms will be presented and used as examples of how these design methods have been (and can be further) utilized to modify existing materials or develop new materials for gas storage and separation applications for environmental and energy related applications including hydrogen, methane, carbon dioxide and hydrocarbon storage or separations.en
dc.language.isoenen
dc.subjectMOFsen
dc.subjectSorptionen
dc.subjectDesignen
dc.subjectMetal organic frameworksen
dc.subjectPorousen
dc.subjectCarbon dioxideen
dc.titleMetal-Organic Frameworks: Building Block Design Strategies for the Synthesis of MOFs.en
dc.typeDissertationen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
thesis.degree.grantorKing Abdullah University of Science and Technologyen_GB
dc.contributor.committeememberPinnau, Ingoen
dc.contributor.committeememberTakanabe, Kazuhiroen
dc.contributor.committeememberZaworotko, Michaelen
thesis.degree.disciplineChemical Sciencesen
thesis.degree.nameDoctor of Philosophyen
dc.person.id102022en
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