(650h) Efficient Formation of C-N Bond and Multi-Carbon Liquid Products in Electrochemical CO Conversion

Using renewable electricity to convert CO to high value products offers an appealing route to store sustainable energy and make use of the chief greenhouse gas CO₂ which can first reduced to CO with high efficiency. Among potential products, chemicals containing carbon–heteroatom bonds such as C-O and C-N are particularly attractive due to their high energy density and industrial relevance. However, significant challenges remain in developing high efficient catalysts and suitable reaction pathway that can selectively produce chemcials at high current densities.

In this talk, we present several strategies to selectively convert CO to C-N bond containing and multi-carbon (C₂₊) liquid products, respectively. A novel CO electro-conversion pathway is designed to achieve over 50% Faradaic efficiencies (FE) and 10 mA cm^-2 current density in C-N bond formation in an H-type electrochemical cell. Catalyst design by tuning the surface CO binding strength shows near 80% FEs and over 100 mA cm^-2 current densities in flow-type electrolyzers. The CO binding strength on catalyst surface is experimental evaluated by developing a surface-enhanced infrared absorption spectroscopic method by measuring CO desorption rates. Density functional theory calculations are employed to obtained more mechanistic insights into these reactions based on the experimental results from our reactivity and spectroscopic combined investigations.