Honors College Thesis
 

Lanthanide Based Metal Organic Framework for the Conversion of CO₂ and Propylene Oxide to Propylene Carbonate

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https://ir.library.oregonstate.edu/concern/honors_college_theses/mg74qt305

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  • Lanthanide (Ln) based molecular complexes have shown great potential as Lewis acid catalysts for the activation of small molecules. Despite the wealth of structural versatility and high catalytic activity of these complexes, they often lack selectivity and recyclability. This hinders their potential for use in large-scale industrial applications where waste minimization is paramount. Herein, we present the use of Ln-based MOFs, Ln(III)HTCPB, as efficient and recyclable catalysts for the conversion of CO₂ into value added products. Propylene carbonate, an important solvent for dyes, batteries, and coating bases, was chosen as a model chemical to be catalyzed by our novel materials. First, propylene epoxide was diffused within the channels of Ce(III)HTCPB where it was found that the epoxide binds to Ce(III) through its O atom—highlighting the active site of the MOF and the activation of the epoxide. Upon CO₂ loading, we found that Ce(III)HTCPB exhibited high catalytic activity with TOF = 20.2 hr⁻¹ and conversion up to 98.5% for the fixation of CO₂ onto propylene oxide into propylene carbonate. The catalyst showed no catalytic deterioration after three cycles and comparable performance in the presence of water and mixed gases (CO₂ mixed with CH₄ or N₂). Catalytic experiments with Ln(III)HTCPB (Ln = Nd, Eu, Tb, Dy, Ho) demonstrated that the rate of CO₂ conversion decreased by decreasing the radii of the Ln used. This study highlights the potential for engineering catalysts via active site size manipulation and for Ln(III)MOFs for CO₂ conversion applications.
  • Key Words: Metal Organic Frameworks, Lanthanides, Epoxides, Cyclic Carbonate, Catalysis, Carbon Dioxide
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  • Pending Publication
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  • 2021-06-03 to 2022-07-03

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