(656f) Advancing the Selective Oxidation of Ethylene Glycol Via Combining Novel Catalyst Design and Density Functional Theory (DFT) Calculations
In this study, a series of monometallic catalysts (including Ag, Pd, Ru, Rd, Fe, Pt) supported on CeO2 were synthesized by using a novel solvothermal method. The oxidation tests were conducted at a mild condition (70 oC, ambient pressure O2) in aqueous alkali solution. The catalysts were characterized by H2 chemisorption, inductively coupled plasma (ICP), transmission electron microscopy (TEM) for the metal content, dispersion and morphology information. Volcano plots of normalized TOF values vs. density functional theory (DFT) calculated Gibbs Free energy was established for EG oxidation. Furthermore, a bimetallic Pt-Fe catalyst showed a significant rate enhancement and selectivity in one-step conversion of EG-to-oxalic acid. The reaction mechanism for EG catalytic oxidation by O2 on (100) and (111) surfaces was studied using DFT calculations which rationalizes the experimental observations that the bimetallic Pt-Fe catalyst has a significantly higher activity (TOF) compared to the monometallic catalysts (Pt and Fe). Fundamental concepts in the computational chemistry and its relation to experimentally observed performance of bimetallic catalysts will be presented in this work.
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