The Influence of Ni Addition in the Mechanism of CO2 Electroreduction on Cu Crystals-Mechanistic Insight from DFT Simulations

Elżbieta Dziadyk-Stopyra; Ionut Tranca; Daniel Smykowski; Bartłomiej M Szyja

doi:10.3390/ma16145138

The Influence of Ni Addition in the Mechanism of CO₂ Electroreduction on Cu Crystals-Mechanistic Insight from DFT Simulations

Materials (Basel). 2023 Jul 21;16(14):5138. doi: 10.3390/ma16145138.

Authors

Elżbieta Dziadyk-Stopyra¹, Ionut Tranca², Daniel Smykowski³, Bartłomiej M Szyja¹

Affiliations

¹ Institute of Advanced Materials, Faculty of Chemistry, Wrocław University of Science and Technology, Gdańska 7/9, 50-344 Wrocław, Poland.
² Algemene Chemie, Vrije Universiteit Brussel, Pleinlaan 2, B-1050 Brussels, Belgium.
³ Department of Energy Conversion Engineering, Faculty of Mechanical and Power Engineering, Wrocław University of Science and Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wrocław, Poland.

Abstract

We present a DFT analysis of the role of the Cu-Ni synergistic effect for the CO₂ reduction to C₂H₄, in comparison to the pure Cu catalyst. The analysis is focused on the thermodynamic stability of reactive intermediates along the proposed pathway of C₂ species formation. We have observed that the potential needed for the reaction decreases with the addition of Ni in the investigated model. In addition, we have observed the differences in the preferred pathway based on the significant differences in stability of the reactive intermediates depending on th Cu:Ni ratio. The results suggest that despite the fact the Cu surface is always exposed, and it is the only one that is able to directly interact with the intermediates, the presence of the Ni in the underlying sections of the crystal is significant enough to change the mechanism of the reaction.

Keywords: CO2 reduction; CuNi; DFT; electrocatalysis; mechanisms.

Grants and funding

This research received no external funding.