English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Electroreduction of CO2 in a Non-aqueous Electrolyte-The Generic Role of Acetonitrile

MPS-Authors
/persons/resource/persons289348

Filser,  Jakob
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons257502

Hörmann,  Nicolas
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22000

Reuter,  Karsten
Theory, Fritz Haber Institute, Max Planck Society;

External Resource
No external resources are shared
Fulltext (restricted access)
There are currently no full texts shared for your IP range.
Fulltext (public)

acscatal.3c00236.pdf
(Publisher version), 4MB

Supplementary Material (public)
There is no public supplementary material available
Citation

Mairegger, T., Li, H., Grießer, C., Winkler, D., Filser, J., Hörmann, N., et al. (2023). Electroreduction of CO2 in a Non-aqueous Electrolyte-The Generic Role of Acetonitrile. ACS Catalysis, 13(9), 5780-5786. doi:10.1021/acscatal.3c00236.


Cite as: https://hdl.handle.net/21.11116/0000-000D-14F3-A
Abstract
Transition metal carbides, especially Mo2C, are praised to be efficient electrocatalysts to reduce CO2 to valuable hydrocarbons. However, on Mo2C in an aqueous electrolyte, exclusively the competing hydrogen evolution reaction takes place, and this discrepancy to theory was traced back to the formation of a thin oxide layer at the electrode surface. Here, we study the CO2 reduction activity at Mo2C in a non-aqueous electrolyte to avoid such passivation and to determine products and the CO2 reduction reaction pathway. We find a tendency of CO2 to reduce to carbon monoxide. This process is inevitably coupled with the decomposition of acetonitrile to a 3-aminocrotonitrile anion. Furthermore, a unique behavior of the non-aqueous acetonitrile electrolyte is found, where the electrolyte, instead of the electrocatalyst, governs the catalytic selectivity of the CO2 reduction. This is evidenced by in situ electrochemical infrared spectroscopy on different electrocatalysts as well as by density functional theory calculations.