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Closing the Loop: Unexamined Performance Trade-Offs of Integrating Direct Air Capture with (Bi)carbonate Electrolysis

Almajed, Hussain M. (author), Kas, Recep (author), Brimley, Paige (author), Crow, Allison M. (author), Somoza Tornos, A. (author), Hodge, Bri Mathias (author), Burdyny, T.E. (author), Smith, Wilson A. (author)

CO₂ from carbonate-based capture solutions requires a substantial energy input. Replacing this step with (bi)carbonate electrolysis has been commonly proposed as an efficient alternative that coproduces CO/syngas. Here, we assess the feasibility of directly integrating air contactors with (bi)carbonate electrolyzers by leveraging...

journal article 2024

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Insertion of MXene-Based Materials into Cu–Pd 3D Aerogels for Electroreduction of CO₂ to Formate

Abdinejad, M. (author), Subramanian, S.S. (author), Motlagh, Mozhgan Khorasani (author), Ripepi, D. (author), Pinto, D. (author), Li, Mengran (author), Middelkoop, J. (author), Urakawa, A. (author), Burdyny, T.E. (author)

The electrochemical CO₂ reduction reaction (CO₂RR) is an attractive method to produce renewable fuel and chemical feedstock using clean energy sources. Formate production represents one of the most economical target products from CO₂RR but is primarily produced using post-transition metal catalysts that...

journal article 2023

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Electroreduction of Carbon Dioxide to Acetate using Heterogenized Hydrophilic Manganese Porphyrins

Abdinejad, M. (author), Yuan, T. (author), Tang, Keith (author), Duangdangchote, Salatan (author), Iglesias van Montfort, H.P. (author), Li, Mengran (author), Middelkoop, J. (author), Wolff, M.J. (author), Burdyny, T.E. (author)

The electrochemical reduction of carbon dioxide (CO₂) to value-added chemicals is a promising strategy to mitigate climate change. Metalloporphyrins have been used as a promising class of stable and tunable catalysts for the electrochemical reduction reaction of CO₂ (CO₂RR) but have been primarily restricted...

journal article 2023

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Creating Conjugated C−C Bonds between Commercial Carbon Electrode and Molecular Catalyst for Oxygen Reduction to Hydrogen Peroxide

Biemolt, J. (author), Meeus, Eva J. (author), de Zwart, Felix J. (author), de Graaf, Jeen (author), Laan, Petrus C.M. (author), de Bruin, Bas (author), Burdyny, T.E. (author), Rothenberg, Gadi (author), Yan, Ning (author)

Immobilizing molecular catalysts on electrodes is vital for electrochemical applications. However, creating robust electrode-catalyst interactions while maintaining good catalytic performance and rapid electron transfer is challenging. Here, without introducing any foreign elements, we show a bottom-up synthetic approach of constructing the...

journal article 2023

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Non-invasive current collectors for improved current-density distribution during CO₂ electrolysis on super-hydrophobic electrodes

Iglesias van Montfort, H.P. (author), Li, Mengran (author), Irtem, I.E. (author), Abdinejad, M. (author), Wu, Yuming (author), Pal, S.K. (author), Sassenburg, M. (author), Ripepi, D. (author), Subramanian, S.S. (author), Biemolt, J. (author), Rufford, Thomas E. (author), Burdyny, T.E. (author)

Electrochemical reduction of CO₂ presents an attractive way to store renewable energy in chemical bonds in a potentially carbon-neutral way. However, the available electrolyzers suffer from intrinsic problems, like flooding and salt accumulation, that must be overcome to industrialize the technology. To mitigate flooding and salt...

journal article 2023

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An Advanced Guide to Assembly and Operation of CO₂ Electrolyzers

Iglesias van Montfort, H.P. (author), Subramanian, S.S. (author), Irtem, I.E. (author), Sassenburg, M. (author), Li, Mengran (author), Kok, J.J. (author), Middelkoop, J. (author), Burdyny, T.E. (author)

journal article 2023

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Effect of Dispersing Solvents for an Ionomer on the Performance of Copper Catalyst Layers for CO₂ Electrolysis to Multicarbon Products

Idros, Mohamed Nazmi (author), Wu, Yuming (author), Duignan, Timothy (author), Li, Mengran (author), Cartmill, Hayden (author), Maglaya, Irving (author), Burdyny, T.E. (author), Wang, Geoff (author), Rufford, Thomas E. (author)

To explore the effects of solvent-ionomer interactions in catalyst inks on the structure and performance of Cu catalyst layers (CLs) for CO₂ electrolysis, we used a “like for like” rationale to select acetone and methanol as dispersion solvents with a distinct affinity for the ionomer backbone or sulfonated ionic heads,...

journal article 2023

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Mapping Spatial and Temporal Electrochemical Activity of Water and CO₂Electrolysis on Gas-Diffusion Electrodes Using Infrared Thermography

Iglesias van Montfort, H.P. (author), Burdyny, T.E. (author)

Electrolysis of water, CO₂, and nitrogen-based compounds presents the opportunity of generating fossil-free fuels and feedstocks at an industrial scale. Such devices are complex in operation, and their performance metrics are usually reported as electrode-averaged quantities. In this work, we report the usage of infrared...

journal article 2022

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Immobilization strategies for porphyrin-based molecular catalysts for the electroreduction of CO₂

Abdinejad, M. (author), Tang, Keith (author), Dao, Caitlin (author), Saedy, S. (author), Burdyny, T.E. (author)

The ever-growing level of carbon dioxide (CO₂) in our atmosphere, is at once a threat and an opportunity. The development of sustainable and cost-effective pathways to convert CO₂ to value-added chemicals is central to reducing its atmospheric presence. Electrochemical CO₂ reduction reactions (CO<sub>2</sub...

journal article 2022

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Electrochemical CO₂ reduction in membrane-electrode assemblies

Ge, Lei (author), Rabiee, Hesamoddin (author), Li, Mengran (author), Subramanian, S.S. (author), Zheng, Yao (author), Lee, Joong Hee (author), Burdyny, T.E. (author), Wang, H. (author)

Electrochemical conversion of gaseous CO₂ to value-added products and fuels is a promising approach to achieve net-zero CO₂ emission energy systems. Significant efforts have been achieved in the design and synthesis of highly active and selective electrocatalysts for this reaction and their reaction mechanism. To perform...

review 2022

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CO₂ Electrolysis via Surface-Engineering Electrografted Pyridines on Silver Catalysts

Abdinejad, M. (author), Irtem, I.E. (author), Farzi, Amirhossein (author), Sassenburg, M. (author), Subramanian, S.S. (author), Iglesias van Montfort, H.P. (author), Ripepi, D. (author), Li, Mengran (author), Middelkoop, J. (author), Seifitokaldani, Ali (author), Burdyny, T.E. (author)

The electrochemical reduction of carbon dioxide (CO₂) to value-added materials has received considerable attention. Both bulk transition-metal catalysts and molecular catalysts affixed to conductive noncatalytic solid supports represent a promising approach toward the electroreduction of CO₂. Here, we report a combined...

journal article 2022

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Mitigating Electrolyte Flooding for Electrochemical CO₂Reduction via Infiltration of Hydrophobic Particles in a Gas Diffusion Layer

Wu, Yuming (author), Charlesworth, Liam (author), Maglaya, Irving (author), Idros, Mohamed Nazmi (author), Li, Mengran (author), Burdyny, T.E. (author), Wang, Geoff (author), Rufford, Thomas E. (author)

Achieving operational stability at high current densities remains a challenge in CO2 electrolyzers due to flooding of the gas diffusion layer (GDL) that supports the electrocatalyst. We mitigated electrode flooding at high current densities using a vacuum-assisted infiltration method to embed 200-400 nm-sized polytetrafluoroethylene (PTFE)...

journal article 2022

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Investigating the role of potassium cations during electrochemical CO₂ reduction

Chandrashekar, S. (author), Iglesias van Montfort, H.P. (author), Bohra, D. (author), Filonenko, G.A. (author), Geerlings, J.J.C. (author), Burdyny, T.E. (author), Smith, W.A. (author)

The specific identity of electrolyte cations has many implications in various electrochemical reactions. However, the exact mechanism by which cations affect electrochemical reactions is not agreed upon in the literature. In this report, we investigate the role of cations during the electrochemical reduction of CO2 by chelating the cations...

journal article 2022

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Energy comparison of sequential and integrated CO₂ capture and electrochemical conversion

Li, Mengran (author), Irtem, I.E. (author), Iglesias van Montfort, H.P. (author), Abdinejad, M. (author), Burdyny, T.E. (author)

Integrating carbon dioxide (CO2) electrolysis with CO2 capture provides exciting new opportunities for energy reductions by simultaneously removing the energy-demanding regeneration step in CO2 capture and avoiding critical issues faced by CO2 gas-fed electrolysers. However, understanding the potential energy advantages of an integrated...

journal article 2022

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Geometric Catalyst Utilization in Zero-Gap CO₂Electrolyzers

Subramanian, S.S. (author), Yang, K. (author), Li, Mengran (author), Sassenburg, M. (author), Abdinejad, M. (author), Irtem, I.E. (author), Middelkoop, J. (author), Burdyny, T.E. (author)

The electrochemical reduction of CO2 (CO2RR) on silver catalysts has been demonstrated under elevated current density, longer reaction times, and intermittent operation. Maintaining performance requires that CO2 can access the entire geometric catalyst area, thus maximizing catalyst utilization. Here we probe the time-dependent factors...

journal article 2022

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Zero-Gap Electrochemical CO₂Reduction Cells: Challenges and Operational Strategies for Prevention of Salt Precipitation

Sassenburg, M. (author), Kelly, Maria (author), Subramanian, S.S. (author), Smith, W.A. (author), Burdyny, T.E. (author)

Salt precipitation is a problem in electrochemical CO2 reduction electrolyzers that limits their long-term durability and industrial applicability by reducing the active area, causing flooding and hindering gas transport. Salt crystals form when hydroxide generation from electrochemical reactions interacts homogeneously with CO2 to generate...

journal article 2022

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Overcoming Nitrogen Reduction to Ammonia Detection Challenges: The Case for Leapfrogging to Gas Diffusion Electrode Platforms

Kolen, M. (author), Ripepi, D. (author), Smith, W.A. (author), Burdyny, T.E. (author), Mulder, F.M. (author)

The nitrogen reduction reaction (NRR) is a promising pathway toward the decarbonization of ammonia (NH3) production. However, unless practical challenges related to the detection of NH3 are removed, confidence in published data and experimental throughput will remain low for experiments in aqueous electrolyte. In this perspective, we analyze...

journal article 2022

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Polymer Modification of Surface Electronic Properties of Electrocatalysts

Venugopal, A. (author), Egberts, Laurentius H.T. (author), Meeprasert, J. (author), Pidko, E.A. (author), Dam, B. (author), Burdyny, T.E. (author), Sinha, V. (author), Smith, W.A. (author)

Finding alternative ways to tailor the electronic properties of a catalyst to actively and selectively drive reactions of interest has been a growing research topic in the field of electrochemistry. In this Letter, we investigate the tuning of the surface electronic properties of electrocatalysts via polymer modification. We show that when a...

journal article 2022

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Characterizing CO2 Reduction Catalysts on Gas Diffusion Electrodes: Comparing Activity, Selectivity, and Stability of Transition Metal Catalysts

Burdyny, T.E. (author), Sassenburg, M. (author), de Rooij, R. (author), Nessbit, Nathan (author), Kas, R. (author), Chandrashekar, S. (author), Firet, N.J. (author), Yang, K. (author), Liu, K. (author), Blommaert, M.A. (author), Kolen, M. (author), Ripepi, D. (author), Smith, W.A. (author)

Continued advancements in the electrochemical reduction of CO 2 (CO 2RR) have emphasized that reactivity,selectivity, and stability are not explicit material properties butcombined effects of the catalyst, double-layer, reaction environ-<br/>ment, and system configuration. These realizations have steadily built upon the foundational work...

journal article 2022

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Advancing integrated CO₂ electrochemical conversion with amine-based CO₂ capture: a review

Li, Mengran (author), Yang, K. (author), Abdinejad, M. (author), Zhao, Chuan (author), Burdyny, T.E. (author)

Carbon dioxide (CO₂) electrolysis is a promising route to utilise captured CO₂ as a building block to produce valuable feedstocks and fuels such as carbon monoxide and ethylene. Very recently, CO₂ electrolysis has been proposed as an alternative process to replace the amine recovery unit of the commercially...

review 2022