Pulsed Electrolysis with a Nickel Molecular Catalyst Improves Selectivity for Carbon Dioxide Reduction.

Pulsed electrolysis can significantly improve carbon dioxide reduction on metal electrodes, but the effect of short (millisecond to seconds) voltage steps on molecular electrocatalysts is largely unstudied. In this work, we investigate the effect pulse electrolysis has on the selectivity and stability of the homogeneous electrocatalyst [Ni(cyclam)] at a carbon electrode. By tuning the potential and pulse duration, we achieve a significant improvement in CO Faradaic efficiencies (85%) after 3 h, double that of the system under potentiostatic conditions.

Zero-Gap Bipolar Membrane Electrolyzer for Carbon Dioxide Reduction Using Acid-Tolerant Molecular Electrocatalysts.

The scaling-up of electrochemical CO reduction requires circumventing the CO loss as carbonates under alkaline conditions. Zero-gap cell configurations with a reverse-bias bipolar membrane (BPM) represent a possible solution, but the catalyst layer in direct contact with the acidic environment of a BPM usually leads to H evolution dominating. Here we show that using acid-tolerant Ni molecular electrocatalysts selective (>60%) CO reduction can be achieved in a zero-gap BPM device using a pure water and CO feed.

Electrochemical carbon dioxide reduction in ionic liquids at high pressure.

Imidazolium ionic liquids are potentially useful solvents for both carbon dioxide reduction conversion and capture. In particular electrocatalytic CO2 reduction has been shown to occur at low overpotentials using a 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ([EMIM][OTf]) and water mixed solvent. A limitation of such solvent systems is their viscosity, making it hard to maintain reasonable catalytic current densities without energy intensive stirring/agitation of the electrolyte.

Continuous and scalable synthesis of a porous organic cage by twin screw extrusion (TSE).

The continuous and scalable synthesis of a porous organic cage (), obtained through a 10-component imine polycondensation between triformylbenzene and a vicinal diamine, was achieved using twin screw extrusion (TSE). Compared to both batch and flow syntheses, the use of TSE enabled the large scale synthesis of using minimal solvent and in short reaction times, with liquid-assisted grinding (LAG) also promoting window-to-window crystal packing to form a 3-D diamondoid pore network in the solid state. A new kinetically trapped [3+5] product was also observed alongside the formation of the targeted [4+6] cage species.