Products Cited in Publications Worldwide Modulation of Selectivity in Electrocatalytic CO2 Reduction with a Magnetic Field and Imidazolium Ionic Liquids

Modulation of Selectivity in Electrocatalytic CO2 Reduction with a Magnetic Field and Imidazolium Ionic Liquids

Karki, Nawaraj; Wilson, Andrew J

DOI:

Abstract

Control over reaction selectivity is among the leading challenges in a wide range of electrocatalytic reactions. Here, we report an approach to tune selectivity in electrocatalytic reactions involving neutrally charged analytes. Using electrocatalytic CO2 reduction in an aqueous medium as a model system, we show that after the interaction of the neutral analyte with an ionic species, the selectivity of CO production over competing H2 production is improved by targeting the mass transport enhancement of charged species using an external magnetic field. Nuclear magnetic resonance spectroscopy and infrared spectroscopy are used to confirm that CO2 can physisorb and chemisorb to imidazolium-based ionic liquids to form charged species. Chronoamperometry and measurements of products with gas chromatography provide evidence that the enhanced transport of charged CO2 complexes induced by an external magnetic field alters reaction selectivity. The reaction selectivity is tunable through the Lorentz force, dependent on the magnetic field strength and current density. Improving the mass transport of CO2 to electrocatalysts with ionic liquids and magnetic fields can improve the energy efficiency of CO2 reduction as well as alter concentration gradients, potentially allowing control over product branching beyond what is possible with electrocatalyst and electrolyte design. The general approach and insights provided in this study are also envisioned to be complementary to electrocatalyst and electrolyte developments for modulating selectivity in electrocatalytic reactions involving neutral species beyond CO2.

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