Reticular Chemistry for the Highly Connected Porous Crystalline Frameworks and Their Potential Applications
KAUST DepartmentPhysical Science and Engineering (PSE) Division
Embargo End Date2019-04-02
Permanent link to this recordhttp://hdl.handle.net/10754/627436
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Access RestrictionsAt the time of archiving, the student author of this dissertation opted to temporarily restrict access to it. The full text of this dissertation became available to the public after the expiration of the embargo on 2019-04-02.
AbstractControl at the molecular level over porous solid-state materials is of prime importance for fine-tuning the local structures, as well as the resultant properties. Traditional porous solid-state materials such as zeolite and activated carbon are the benchmarks in the current market with vital applications in sorption and heterogeneous catalysis. However, the adjustments of pore size and geometry of those materials, which are essential for the broader aspect of modern prominent applications, remain challenging. Reticular chemistry has emerged as a dominant tool toward the ‘designed syntheses’ of porous crystalline frameworks (e.g. metal-organic frameworks (MOFs)) with a specific pore system. This dissertation illustrates the power of reticular chemistry and its use in the directional assembly of highly coordinated MOF materials, as well as their potential applications such as gas storage, natural gas upgrading, and light hydrocarbon separation. Highly connected minimal edge-transitive derived and related nets, obtained via the deconstruction of nodes of the edge-transitive nets, are suitable blueprints and can potentially be deployed in the future ‘designed syntheses’ of MOFs. The further employment of the conceptual net-coded building units (e.g. highly connected MBBs and edge-transitive SBLs) in the practical reticular synthesis results in the rational design and construction of functional MOF platforms like shp-, alb-, kce-, kex- and eea- MOFs. In addition, the isoreticular synthesis of Al-cea-MOF-2 with functionalized pendant acid moieties inside pore channels in comparison to the parent Al-cea-MOF-1 led to enhanced light hydrocarbons separation performance. Moreover, controlling the molecular defects in Zr-fum-fcu-MOFs resulted in the development of an ultramicroporous adsorbent with an engineered aperture size for the highly efficient separation of butane/iso-butane.