Investigation of Metal Organic Frameworks for Renewable Energy Electrocatalysis

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Catalyst development*for renewable energy utilization is a pressing global issue. The goal for my*research program is to investigate electrocatalytic metal organic frameworks*(MOFs) with rationally designed three dimensional catalytically active pockets*for conversion of electricity to fuels and chemicals. My objective is to*demonstrate that efficiently driving reactions from CO2 and H2O*starting materials to the desired products (i.e. CH3OH, CH4,*CH3CH2OH) can be accomplished by establishing MOF-based*electrochemical systems that incorporate enzyme-inspired reaction effects.*These include intermediate stabilization, proton relays, and multiple reactant*binding sites within the confined, molecularly tunable catalytic environments*of the MOFs. An example is the use of a MOF functionalized with amino groups to*stabilize high energy intermediates through hydrogen-bonding interactions and*flatten the reaction free energy landscape to accelerate catalysis. Longer term (3-5*year) goals include incorporating proximal active sites to facilitate reactant*dimerization to drive the reaction pathway towards C2 products*from CO2. In addition, the invesitgation of nanoparticle@MOF*core@shell materials will be undertaken. Such systems allow for independent*tuning of a nanoparticle catalytically active surface and the immediate*reaction environment conferred by the MOF shell.***By utilizing*the porous MOFs as molecularly tunable electrocatalytic materials, the*strengths of heterogeneous (tuneability) and homogeneous (activity, stability)*catalysts are combined while also incorporating a new bio-inspired element into*the research. To realize the proposed materials, my research team will*construct MOF-electrodes by growing MOF thin films directly on conductive*substrates. These MOF electrodes will be used directly to catalyze CO-2 reduction*in an aqueous electrochemical cell. Their activity and selectivity will be*evaluated with electrochemical methods and with a combination of gas*chromatography and NMR to detect reaction products. In tandem to synthesis and*characterization of MOF electrocatalysts,