Work

Electrochemical CO Reduction: A Property of the Electrochemical Interface

Year: 2019

Type: article

Abstract: Electrochemical CO reduction holds the promise to be a cornerstone for sustainable production of fuels and chemicals. However, the underlying understanding of the carbon-carbon coupling toward multiple-carbon products is not complete. Here we present thermodynamically realistic structures of the electrochemical interfaces, determined by explicit ab initio simulations. We investigate how key CO reduction reaction intermediates are stabilized in different electrolytes and at different pH values. We find that the catalytic trends previously observed experimentally can be explained by the interplay between the metal surface and the electrolyte. For the Cu(100) facet with a phosphate buffer electrolyte, the energy efficiency is found to be limited by blocking of a phosphate anion, while in alkali hydroxide solutions (MOH, M = Na, K, Cs), OH* intermediates may be present, and at high overpotential the H* coverage limits the reaction. The results provide insight into the electrochemical interface structure, revealing the limitations for multiple-carbon products, and offer a direct comparison to experiments.

Source: Journal of the American Chemical Society

DOI: 10.1021/jacs.8b08839

Authors: Alexander Bagger, Logi Arnarson, Martin H. Hansen, Eckhard Spohr, Jan Rossmeisl

Institutions: University of Copenhagen, SLAC National Accelerator Laboratory, University of Duisburg-Essen

Language: English

Topic: CO2 Reduction Techniques and Catalysts

Subfield: Renewable Energy, Sustainability and the Environment

Field: Energy

Domain: Physical Sciences

SDG: Affordable and clean energy

Open Access status: green

Funders: Innovationsfonden, Carlsbergfondet