Date/Time
23.01.2025
2:00 pm – 3:00 pm
Location
Lecture Hall 55.02
Pfaffenwaldring 55
70569 Stuttgart
We are very happy to welcome within the CRC 1333 Colloquium Series:
Thursday, January 23, 2025, 2:00-3:00 pm
Department of Chemistry, Nanoscience Center
University of Jyväskylä Finland
Topic: “Exploring cation-induced changes CO2 reduction on Au using advanced
computational approaches”
Abstract:
Recent experimental studies have highlighted the significant influence of cations on the CO2
reduction reaction (CO2RR), though their precise role remains elusive. In this talk, I will
present our recent computational findings1 on cation effects in CO2RR. Using constrained
density functional theory (DFT) molecular dynamics and slow-growth DFT molecular
dynamics, we simulated both outer-sphere (OS-ET) and inner-sphere electron transfer (IS-ET)
pathways.
Our results indicate that in the absence of cations, only the OS-ET pathway is feasible, with
an energy barrier of 1.21 eV. However, the presence of K+ or Li+ cations dramatically increases
the OS-ET barrier to 2.93 eV and 4.15 eV, respectively, rendering this process energetically
prohibitive. Conversely, cations facilitate the IS-ET pathway, lowering the barrier to 0.61 eV
for K+ and 0.91 eV for Li+, with adsorbed CO2δ- as a key intermediate. Without cations, the
transition from solvated CO2 to adsorbed CO2δ- does not occur.
These findings suggest that cation effects, driven by short-range Coulomb interactions with
intermediates, can enhance CO2RR activity and Faradaic efficiency, provided their
concentration remains optimal.
References:
1. X. Qin, et al. Nat. Comm. 14, 7607 (2023) Cation-induced changes in the inner- and
outer-sphere mechanisms of electrocatalytic CO2 reduction
The CRC cordially invites all who are interested to the lecture.