Browsing by Author "Elias, Welman C."

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    Impregnation of KOAc on PdAu/SiO2 causes Pd-acetate formation and metal restructuring
    (Royal Society of Chemistry, 2023) Jacobs, Hunter P.; Elias, Welman C.; Heck, Kimberly N.; Dean, David P.; Dodson, Justin J.; Zhang, Wenqing; Arredondo, Jacob H.; Breckner, Christian J.; Hong, Kiheon; Botello, Christopher R.; Chen, Laiyuan; Mueller, Sean G.; Alexander, Steven R.; Miller, Jeffrey T.; Wong, Michael S.; Chemical and Biomolecular Engineering; Chemistry; Civil and Environmental Engineering; Materials Science and Nanoengineering
    Potassium-promoted, oxide-supported PdAu is catalytically active for the gas-phase acetoxylation of ethylene to form vinyl acetate monomer (VAM), in which the potassium improves long-term activity and VAM selectivity. The alkali metal is incorporated into the catalyst via wet impregnation of its salt solution, and it is generally assumed that this common catalyst preparation step has no effect on the catalyst structure. However, in this work, we report evidence to the contrary. We synthesized a silica-supported PdAu (PdAu/SiO2, 8 wt% Pd, 4 wt% Au) model catalyst containing Pd-rich PdAu alloy and pure Au phases. Impregnation with potassium acetate (KOAc) aqueous solution and subsequent drying did not cause XRD-detectible changes to the bimetal structure. However, DRIFTS indicated the presence of Pd3(OAc)6 species, which is correlated to up to 2% Pd loss after washing of the dried KOAc-promoted PdAu/SiO2. Carrying out the impregnation step with an AcOH-only solution and subsequent drying caused significant enlargement of the pure Au grain size and generated a smaller amount of Pd3(OAc)6. During co-impregnation of AcOH and KOAc, grain sizes were enlarged slightly, and substantial amounts of K2Pd2(OAc)6 and Pd3(OAc)6 were detected by DRIFTS and correlated to up to 32% Pd loss after washing. Synchrotron XAS analysis showed that approximately half the Pd atoms were oxidized, corroborating the presence of the Pd-acetate species. These results indicate wet-impregnation-induced metal leaching can occur and be substantial during catalyst preparation.
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    A Simple and Rapid Method of Forming Double-Sided TiO2 Nanotube Arrays
    (Wiley, 2022) Conrad, Christian L.; Elias, Welman C.; Garcia-Segura, Sergi; Reynolds, Michael A.; Wong, Michael S.; Chemical and Biomolecular Engineering; Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment
    Highly ordered TiO2 nanostructures, known as nanotube arrays (NTAs), exhibit potential in various energy, chemical sensing, and biomedical applications. Owing to its simplicity and high degree of control, titanium anodization serves as the prevailing NTA synthesis method. However, the practicality of this approach is marred by sluggish and inconsistent growth rates, on the order of 10 nm min−1. Growth rates strongly depend on the electrolyte conductivity, yet most reports neglect to consider this property as a measured and controllable parameter. Here, we have systematically determined a broad set of conditions (at 60 V applied potential, elevated temperatures) that allow researchers to fabricate NTAs quickly and simply. By modulating conductivity through variation of bulk electrolyte temperature and the controlled addition of several hydroxy acid species, we achieve consistent accelerated growth up to 10 times faster than traditional methods. We find that regulating the solution conductivity within a desired region (e. g., ∼800–1000 μS cm−1) enabled the fabrication of double-sided NTA layers of around 10 μm and 90 μm NTA in 10 and 180 min, respectively.