The scaling-up of
electrochemical CO2 reduction requires
circumventing the CO2 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 H2 evolution dominating. Here we show that using acid-tolerant
Ni molecular electrocatalysts selective (>60%) CO2 reduction
can be achieved in a zero-gap BPM device using a pure water and CO2 feed. At a higher current density (100 mA cm–2), CO selectivity decreases, but was still >30%, due to reversible
product inhibition. This study demonstrates the importance of developing
acid-tolerant catalysts for use in large-scale CO2 reduction
devices.
The melting and glass-forming behaviour of a range of organic cages was investigated, with quenching of melted liquid states providing molecular glasses, one of which exhibited improved gas uptake compared to the starting amorphous cage.
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...
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)]2+ 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.
The improved activity is due to in situ catalyst regeneration from
an intermediate that occurs as part of the catalyst’s degradation
pathway. This study demonstrates the wider opportunity to apply pulsed
electrolysis to molecular electrocatalysts to control activity and
improve selectivity.
The scaling-up of electrochemical CO2 reduction requires circumventing the CO2 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 H2 evolution dominating. Here we show that using acid-tolerant Ni molecular electrocatalysts selective (> 60%) CO2 reduction can be achieved in a zero-gap BPM device using a pure water and CO2 feed. At higher current density (100 mA cm-2), CO selectivity de-creases, but was still >30%, due to reversible product inhibition. This study demonstrates the importance of developing acid-tolerant catalysts for use in large-scale CO2 reduction devices.
The continuous and scalable synthesis of a porous organic cage (<b>CC3</b>), 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 <b>CC3</b> 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. Post-synthetic purification by Soxhlet extraction of the as-extruded ‘technical grade’ mixture of <b>CC3</b> and [3+5] species rendered the material porous.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.