Elucidating the Effect of Sorbent-Enhanced CO2 Availability for Electroreduction: from Model System to Membrane Electrode Assembly

Marieke van Leeuwen^a^,^b^,^c, Martijn J. W. Blom^a^,^b^,^c, Nina Plankensteiner^a^,^b^,^c, Alan C. West^d, Philippe M. Vereecken^a^,^b^,^c

^acMACS Department of Microbial and Molecular Systems, KU Leuven, Belgium, Kasteelpark Arenberg 23, Leuven, Belgium

^bimec Leuven, Belgium, Remisebosweg, 1, Leuven, Belgium

^cEnergyVille, Thor Park 8320, B-3600 Genk, Belgium

^dColumbia University, US, Broadway, 3000, New York, United States

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

Oral, Marieke van Leeuwen, presentation 249
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.249
Publication date: 28th August 2024

Local CO₂ availability at the catalyst is an important limitation for low temperature CO₂ electroreduction in aqueous media. Integrated CO₂ capture and electrochemical utilization is energetically and economically advantageous, as it combines sorptive and electrolytic functions [1]. Previously chemicals used as sorbent and organic electrolyte include monoethanolamine and ionic liquids [2]. Improved uptake capacity, kinetics, and selectivity as well as good chemical and thermal stability are essential criteria in the sorbent electrolyte selection process [3]. A common employed strategy to overcome the mass transport-limited CO₂ supply in liquid electrolyte systems is to provide CO₂ in its gaseous form to the electrode, leading to record performances in such systems [4].

Integration of sorbents in gas-fed electrolyzers enables to locally increase CO₂ availability and thereby boost the maximum reduction rate [5]. Typical Membrane Electrode Assembly (MEA) designs are composed of multiple layers (e.g., hydrophobic porous transport layer, carbon nanoparticles or fibers, ionomer, catalyst nanoparticles, …). Studying the effect of the sorbent and its integration in the assembly is impeded by the stack complexity and therefore hard to decouple from other phenomena. In this work, a planar interdigitated electrode assembly was developed to test sorbent electrolytes for CO₂ reduction in gas-fed environments under well-defined conditions. Ionic liquid-silica nanocomposites were successfully tested as sorbent electrolyte coatings for CO₂ reduction in such a gas-fed model system, providing a proof-of-concept for the enhanced CO₂ electroreduction by increasing reactant availability . Next to the experimental approach, kinetic parameters for the CO₂ uptake, transport and electroreduction were modeled in a multiphysics model and compared to experiments. The extracted kinetic parameters obtained from the interdigitated electrode model system were implemented in a model of a MEA configuration to determine optimum sorbent placement.

References:

[1] I. Sullivan et al., “Coupling electrochemical CO2 conversion with CO2 capture,” Nat. Catal., vol. 4, no. 11, Art. no. 11, Nov. 2021

[2] E. Pérez-Gallent, C. Vankani, C. Sánchez-Martínez, A. Anastasopol, and E. Goetheer, “Integrating CO2 Capture with Electrochemical Conversion Using Amine-Based Capture Solvents as Electrolytes,” Ind. Eng. Chem. Res., vol. 60, no. 11, pp. 4269–4278, Mar. 2021

[3] B. B. Polesso et al., “Imidazolium-based Ionic Liquids Impregnated in Silica and Alumina Supports for CO2 Capture,” Mater. Res., vol. 22, no. suppl 1, p. e20180810, 2019

[4] Á. Vass, A. Kormányos, Z. Kószó, B. Endrődi, and C. Janáky, “Anode Catalysts in CO2 Electrolysis: Challenges and Untapped Opportunities,” ACS Catal., vol. 12, no. 2, pp. 1037–1051, Jan. 2022

[5] D.-H. Nam et al., “High-Rate and Selective CO2 Electrolysis to Ethylene via Metal–Organic-Framework-Augmented CO2 Availability,” Adv. Mater., vol. 34, no. 51, p. 2207088, 2022

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