Electrolyte-Guided Design of Electroreductive CO Coupling on Copper Surfaces

Authors
Akhade,
Sneha A.,
Jayathilake,
Buddhinie S.,
Weitnzer,
Stephen E.,
Eshelman,
Hannah V.,
Hamilton,
Julie,
Feaster,
Jeremy T.,
Wakerley,
David W.,
Wang,
Lei,
Lamaison,
Sarah,
Lee,
Dong Un,
Hahn,
Christopher,
Jaramillo,
Thomas F.,
Duoss,
Eric B.,
Baker,
Sarah E.,
Varley,
Joel B.
Year of publication
2021
Journal
ACS Applied Energy Materials
Issue
8
Volume
4
Starting page
8201
Ending page
8210
Engineering the interfacial distribution of electrolytic ions can aid in modulating the electrocatalyst performance and efficiency. Using a hybrid quantum-classical modeling approach, we describe how predictive tuning of the solution microenvironment on copper can enhance the efficiency of CO2 reduction (CO2R) to C2 products. We elucidate how competing electrolyte constituents in mixed electrolyte solutions stimulate restructuring of the electrochemical double layer (EDL) and stabilize the OCCO* dimer (* denotes surface adsorbed), with predictions validated in flow reactors using copper gas diffusion electrodes (Cu-GDEs). Our findings highlight how molecular-scale electrolyte engineering with informed models of the EDL can be leveraged to tailor CO2R activity and selectivity toward C2 products.
Funding sources