(532ab) Understanding the Mechanism of C-N Coupling in Electrochemical CO2 Reduction on Metal Surfaces | AIChE

(532ab) Understanding the Mechanism of C-N Coupling in Electrochemical CO2 Reduction on Metal Surfaces


Han, X., Virginia Tech
Zhu, H., Virginia Tech Chemical Engineering
Xin, H., Virginia Tech
Carbon neutrality is essential for achieving sustainable development of human societies. Among various technologies of carbon conversion, electrochemical CO2 reduction has drawn attention since it has the potential to solve the greenhouse gas issue and potentially store the intermittent renewable energy to chemicals. The state-of-the-art electrocatalytic CO2 reduction usually produces a variety of carbon-based products. However, it’s hard to further increase the value and expand the scope of products which is limited by solely employing CO2 and H2O as reactants. The integration of N into the electrochemical CO2 reduction could offer valuable products including organonitrogen compounds when considering the bond-forming between carbon and nitrogen. The C-N coupling induced electrochemical CO2 reduction is environmentally and economically beneficial since it could yield organonitrogen compounds which are normally sourced from NH3 industrially produced by the energy extensive Haber-Bosch process. Nonetheless, the complicated reaction mechanism of C-N coupling in CO2 reduction remains elusive due to the multistep kinetics and unclear C-N coupling intermediates. Supported by in-situ experimental measurements and characterizations, we performed theoretical studies to unravel the mechanism of C-N coupling in electrocatalytic CO2 reduction starting from CO2 and NO3- reactants on metal surfaces. By employing the chemisorption and machine learning (ML) models, we also performed the rational design for catalysts candidates that show promising performance, which opens a new path for catalytic materials discovery for organonitrogen compound production.