Operando Probing of Cu Surfaces during the Electrochemical CO Reduction Reaction with X-ray Photoelectron Spectroscopy

Bernadette Davies^a, Sara Boscolo-Bibi^b, Fernando Garcia-Martinez^c, Sergey Koroidov^b

^aDepartment of Materials and Environmental Chemistry, Stockholm University, Sweden

^bDepartment of Physics, Stockholm University

^cPhoton Science, Deutsches Elektronen-Synchrotron (DESY), Hamburg 22607, Germany

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)

#CO2X - Frontier developments in Electrochemical CO2 reduction and the utilization

Torremolinos, Spain, 2023 October 16th - 20th

Organizers: Alexander Bagger and Yu Katayama

Poster, Bernadette Davies, 335
Publication date: 18th July 2023

Copper is the only known material able to achieve electrochemical reduction of CO₂ and CO to valuable C2+ products.[1] However, many aspects of the mechanism are disputed and many mechanistic studies on Cu are purely computational. Well designed operando mechanistic studies are vital to fill this gap. We are developing a methodology for probing electrochemical reactions operando using the ambient pressure X-ray photoelectron spectroscopy (APXPS) instrument POLARIS at DESY, specialized towards measuring XPS at advanced pressures.[2]

To be able to make CO/CO₂ conversion to fuels and chemical feedstocks industrially viable, it is vital to be able to control the selectivity towards a smaller distribution of more valuable products. It is well known that Cu single crystals with a greater density of step sites produce a more favourable ratio of ethylene over methane.[3] The aim of this project is to study the differences in the electrochemical CO reduction mechanism on Cu(100), Cu(111) and Cu(711) single crystals with operando APXPS, to develop understanding of the mechanism and how different single crystal facets influence the selectivity.

References:

[1] Ma, W. et al. Electrocatalytic reduction of CO2and CO to multi-carbon compounds over Cu-based catalysts. Chem. Soc. Rev. 50, 12897–12914 (2021).

[2] Degerman, D. et al. Operando X-ray Photoelectron Spectroscopy for High-Pressure Catalysis Research Using the POLARIS Endstation. Synchrotron Radiat. News 35, 11–18 (2022).

[3] Nitopi, S. et al. Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte. Chem. Rev. 119, 7610–7672 (2019).

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