TY - JOUR
T1 - A Cation Concentration Gradient Approach to Tune the Selectivity and Activity of CO2 Electroreduction
AU - Ren, Wenhao
AU - Xu, Aoni
AU - Chan, Karen
AU - Hu, Xile
N1 - Publisher Copyright:
© 2022 Wiley-VCH GmbH.
PY - 2022
Y1 - 2022
N2 - The linear scaling relationship of the binding energies of different intermediates limits the catalyst performance in CO2 electroreduction. Here we demonstrate a cation concentration gradient strategy to promote the activity and tune the selectivity of CO2 electroreduction, thereby breaking the scaling relationship. In optimal concentrations of the potassium acetate (KAc) electrolyte, Cu, Ag and In catalysts deliver current densities that are 7.1, 3.2, 2.7 times higher than those obtained in 0.5 M KAc for C2H4, CO, and formate production, respectively. Increasing the concentration of KAc also changes the selectivity from CO to formate on Ag, and from CO to C2 products on Cu. In situ surface-enhanced Raman spectroscopy and computational simulations reveal that the binding energies of intermediates are changed at different electrolyte concentrations, which is due to a local electrostatic interaction modulated by potassium cations at the electrode surface.
AB - The linear scaling relationship of the binding energies of different intermediates limits the catalyst performance in CO2 electroreduction. Here we demonstrate a cation concentration gradient strategy to promote the activity and tune the selectivity of CO2 electroreduction, thereby breaking the scaling relationship. In optimal concentrations of the potassium acetate (KAc) electrolyte, Cu, Ag and In catalysts deliver current densities that are 7.1, 3.2, 2.7 times higher than those obtained in 0.5 M KAc for C2H4, CO, and formate production, respectively. Increasing the concentration of KAc also changes the selectivity from CO to formate on Ag, and from CO to C2 products on Cu. In situ surface-enhanced Raman spectroscopy and computational simulations reveal that the binding energies of intermediates are changed at different electrolyte concentrations, which is due to a local electrostatic interaction modulated by potassium cations at the electrode surface.
KW - CO2Reduction
KW - Cation Effect
KW - Concentration Gradient
KW - Electrocatalysis
U2 - 10.1002/anie.202214173
DO - 10.1002/anie.202214173
M3 - Journal article
C2 - 36239987
AN - SCOPUS:85141656518
VL - 61
JO - Angewandte Chemie International Edition
JF - Angewandte Chemie International Edition
SN - 1433-7851
IS - 49
M1 - e202214173
ER -