Activating New Reaction Pathways in Electrochemical CO2 Conversion Using Pulsing
Matthew T. Mayer a, Alexander Arndt a, Laura C. Pardo Pérez a, Chaoqun Ma a
a Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Berlin, Germany
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
#PECCO2 - Advances in (Photo)Electrochemical CO2 Conversion to Chemicals and Fuels
Lausanne, Switzerland, 2024 November 12th - 15th
Organizers: Deepak PANT, Adriano Sacco and juqin zeng
Invited Speaker, Chaoqun Ma, presentation 245
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.245
Publication date: 28th August 2024

Electrochemical CO2 conversion can result in a variety of products, often as a mixture, and controlling the product selectivity remains a key challenge. It has been shown that pulsing the electrochemical potential can lead to altered product distributions, influenced by effects on, e.g., transport, double-layer rearrangement, adsorption/desorption, and changes to electrode structure and composition [1].

Herein we report our observations using metal electrodes normally selective for the 2-electron formation of CO as major product under steady-state (potentiostatic) conditions, finding that they can produce significant amounts of higher-order products (including methane and ethylene) under the application of pulse potential waveforms. We confirm this is not due to metal impurities in the system, but is significantly affected by phenomena such as surface restructuring and accumulation of liquid products. Furthermore, time-resolved differential electrochemical mass spectrometry (DEMS) measurements reveal distinctly different transient behaviors between the different gaseous products, providing key new mechanistic insight for clarifying the roles of pulsing.

Helmholtz Association's Initiative and Networking Fund (Helmholtz Young Investigator Group VH-NH-1225). Deutsche Forschungsgemeinschaft (DFG, German Research 
Foundation) – Projektnummer 501805371.

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