Oxide-Encapsulated Silver Electrocatalysts for Selective and Stable Syngas Production from Reactive Carbon Capture Solutions.

Electrolysis of bicarbonate-containing CO capture solutions is a promising approach towards achieving low-cost carbon-neutral chemicals production. However, the parasitic bicarbonate-mediated hydrogen evolution reaction (HER) and electrode instability in the presence of trace impurities remain major obstacles to overcome. This work demonstrates that the combined use of titanium dioxide (TiO) overlayers with the chelating agent ethylene diamine tetra-acetic acid (EDTA) significantly enhances the selectivity and stability of Ag-based electrocatalysts for bicarbonate electrolysis.

Condensed Layer Deposition of Nanoscopic TiO Overlayers on High-Surface-Area Electrocatalysts.

Encapsulating an electrocatalytic material with a semipermeable, nanoscopic oxide overlayer offers a promising approach to enhancing its stability, activity, and/or selectivity compared to an unencapsulated electrocatalyst. However, applying nanoscopic oxide encapsulation layers to high-surface-area electrodes such as nanoparticle-supported porous electrodes is a challenging task. This study demonstrates that the recently developed condensed layer deposition (CLD) method can be used for depositing nanoscopic (sub-10 nm thick) titanium dioxide (TiO) overlayers onto high-surface-area platinized carbon foam electrodes.

Unraveling Unique Surface Chemistry of Transition Metal Nitrides in Controlling Selective C-O Bond Scission Pathways of Glycerol.

Controlled C-O bond scission is an important step for upgrading glycerol, a major byproduct from the continuously increasing biodiesel production. Transition metal nitride catalysts have been identified as promising hydrodeoxygenation (HDO) catalysts, but fundamental understanding regarding the active sites of the catalysts and reaction mechanism remains unclear. This work demonstrates a fundamental surface science study of MoN and Cu/MoN for the selective HDO reaction of glycerol, using a combination of model surface experiments and first-principles calculations.

Controlling reaction pathways of selective C-O bond cleavage of glycerol.

The selective hydrodeoxygenation (HDO) reaction is desirable to convert glycerol into various value-added products by breaking different numbers of C-O bonds while maintaining C-C bonds. Here we combine experimental and density functional theory (DFT) results to reveal that the Cu modifier can significantly reduce the oxophilicity of the molybdenum carbide (MoC) surface and change the product distribution. The MoC surface is active for breaking all C-O bonds to produce propylene.