Synthesis strategies towards new heterometallic and functionalized MOFs
(2022)
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- Metal-organic frameworks (MOFs) are porous coordination tri-dimensional assemblies with potential use for many applications, and especially in catalysis, gas storage and adsorption from solution. The work presented in this thesis mainly aims at improving the sustainable production of MOFs containing trimesate linkers, with well-characterized structures, as well as at the introduction of new types of active sites, under the form of second (“exotic”) metals, amine functions and defects, by easy to implement synthetic approaches. The main part of this thesis concerns the development of a new green aqueous strategy for obtaining the mesoporous MOF MIL 100(Fe) through the use of alkali trimesate salts and the investigation of the MOF’s formation mechanism. This synthetic strategy was further developed to allow incorporation of a second metal to obtain bimetallic MIL 100(Fe,M) incorporating transition, p-bloc and rare-earth elements as secondary metals in a one-pot fashion. The functionalization of mono- and bimetallic Al- and Fe-based MIL 100 MOFs with ethylenediamine (EN) was also investigated, including the CO2 adsorption performances and possibility to post-functionalize the obtained materials. Synthetic efforts were also made to improve the sustainability of the synthesis of lanthanide-based MOF 76 metal-organic frameworks, and increasing their stability towards water by linker modification. Finally, the synthesis of a new type of TiIII-based MOF, NH2 MIL 101(TiIII), was achieved, and the introduction of structural defects induced by mechanosynthesis was studied on HKUST 1 as model MOF. The new materials obtained in this work may find use in multiple applications, such as catalysis and gas sorption.
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Steenhaut, T. (2022). Synthesis strategies towards new heterometallic and functionalized MOFs. https://hdl.handle.net/2078.5/249035