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    Synthesis and Characterization of Transition Metal Ion-based Hydrogels with Auxiliary Carboxylate Spacer Ligands for Selective Carbon Dioxide Separation and Other Potential Applications

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    Name:
    Mona Aldossary - Final Paper.pdf
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    Description:
    Mona Aldossary - Final Paper
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    Type
    Dissertation
    Authors
    Al Dossary, Mona cc
    Advisors
    Hadjichristidis, Nikos cc
    Committee members
    Saikaly, Pascal cc
    Cavallo, Luigi cc
    Khushaim, Muna S. cc
    Program
    Chemical Science
    KAUST Department
    Physical Science and Engineering (PSE) Division
    Date
    2018-11
    Permanent link to this record
    http://hdl.handle.net/10754/630121
    
    Metadata
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    Abstract
    Metallo-supramolecular hydrogels have interesting dynamic properties for many applications. We report a simple method for synthesizing copper-based polymer hydrogels made from nontoxic poly(methyl vinyl ether-alt-maleic anhydride) (PVM-alt-MA) in the absence or presence of added dicarboxylates, such as adipate and terephthalate. We utilize metal-polycarboxylate backbone and carboxylate spacer ligands between polymers strands engineered via non-covalent metal ion coordination. Rheological measurements revealed that the mechanical stability of the hydrogels was enhanced by the addition of supplementary dicarboxylate ligands. The optimal ratio of polymer to dicarboxylate to Cu2+ was 10:4:2.5. Our scanning electron microscope (SEM) and Cryo-SEM imaging and physical adsorption measurements revealed the formation of pores. The Brunauer–Emmett–Teller (BET) surface area of the dried hydrogels increased from 177.96 m2 g−1 in a dried hydrogel without added dicarboxylate to 646.90 and 536.44 m2 g−1 with the addition of adipate and terephthalate, respectively. The pore volume increased as well. Separation of CO2 from post-combustion flue gases is important for environmental and economic sustainability. The PVM-alt-Na-MA:adipate:Cu2+ hydrogels are promising material for post-combustion CO2 separation. At normal conditions (298 K and 1 bar), the PVM-alt-Na-MA:adipate:Cu2+ hydrogel samples with 10:4:2.5 ratio, showed notable CO2/N2 selectivity of 78.46 and a high CO2/CH4 selectivity reaching 26.09 at 1 bar. Additionally, we investigated in detail the effect of transition metal ion on the rigidity and structure of hydrogels using Al3+, Fe3+, Cu2+, Ni2+, Zn2+, and Co2+. We also studied the effect of using tricarboxylate spacer ligands such as nitrilotriacetic (NTA) and trisodium citrate or tetracarboxylate such as ethylenediaminetetraacetic acid (EDTA). It is important to mention that one of the main advantages of our facile synthesis method is being simple and can be scaled up for commercial applications. For scaling up the synthesis of hydrogels, we utilized a filling machine that is able to increase the amount of hydrogel aliquots with variable volume. Silver-based hydrogels showed significant antibacterial activity, due to the presence of silver nanoparticles. We utilized a filling machine for application of amorphous wound dressing. The optimization of the conditions of the filling enabled us to scale up the synthesis and the filling process.
    Citation
    Al Dossary, M. (2018). Synthesis and Characterization of Transition Metal Ion-based Hydrogels with Auxiliary Carboxylate Spacer Ligands for Selective Carbon Dioxide Separation and Other Potential Applications. KAUST Research Repository. https://doi.org/10.25781/KAUST-123R0
    DOI
    10.25781/KAUST-123R0
    ae974a485f413a2113503eed53cd6c53
    10.25781/KAUST-123R0
    Scopus Count
    Collections
    Dissertations; Physical Science and Engineering (PSE) Division; Chemical Science Program

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