Electrochemical CO2 reduction reaction: Altering selectivity with atomic layer deposition
Benjamin Bowers a, Yuxiang Zhou a, Rose Oates a, Ludmilla Steier b, Ifan Stephens a
a Materials Department, Imperial College London
b University of Oxford, Department of Chemistry, Oxford, OX1 3TA, United Kingdom
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
Oral, Benjamin Bowers, presentation 190
DOI: https://doi.org/10.29363/nanoge.matsus.2023.190
Publication date: 18th July 2023

Electrochemical CO2 reduction reaction, is the conversion of CO2 to products through the application of charge in an electrolysis cell. If CO2 could be selectively converted to a particular high value product at low overpotential and high current density, CO2 would be turned into an energy storage molecule and/or a chemical feedstock, driving society closer to closing the carbon loop.

Since the early-mid 90s, research into CO2 reduction reaction materials has primarily centred around copper1-3.  Copper has the unique ability to bind to key intermediates *CO and H* moderately4, improving the chance of hydrogenation or coupling reaction steps5. Incremental improvements in cell design and nano structuring have improved the partial current density towards high value C2+ products. Size control6, oxide derived copper7 and facets8 among others effects have been tested, but questions remain whether the intrinsic activity towards the CO2 reduction reaction on copper has been improved. A possible work around, is to alter the localized concentration of key intermediates. Therefore, multiple groups have paired Cu with a secondary, CO producing active site, to form a tandem mechanism9-11.

In this talk I will be highlighting the advantages of using atomic layer deposition (ALD) in electrocatalysis and how it can form a method towards altering selectivity for the CO2 reduction reaction.  I will initially present the requirement for altering copper activity through relating activity towards CO2 reduction reaction to surface roughness of nanostructured copper and oxide-derived copper. Subsequently, trends in selectivity with different metal oxide nanoclusters atop copper nanoparticles are shown towards the CO2 reduction reaction, with CO reduction reaction being used as a mechanistic tool. Further characterization techniques both ex and in situ will be presented to shed light on the changes in selectivity including XPS, in-situ contact angle measurements and FTIR amongst others.

 

EPSRC Doctoral Training Partnership (DTP)

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