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A Quantitative Analysis of Electrochemical CO2 Reduction on Copper in Organic Amide and Nitrile-Based Electrolytes

Sajeev Kumar, A. (author), Moura de Salles Pupo, M. (author), Petrov, K.V. (author), Ramdin, M. (author), van Ommen, J.R. (author), de Jong, W. (author), Kortlever, R. (author)

Aqueous electrolytes used in CO2 electroreduction typically have a CO2 solubility of around 34 mM under ambient conditions, contributing to mass transfer limitations in the system. Non-aqueous electrolytes exhibit higher CO2 solubility (by 5–8-fold) and also provide possibilities to suppress the undesired hydrogen evolution reaction (HER). On...

journal article 2023

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Revisiting the Electrochemical Nitrogen Reduction on Molybdenum and Iron Carbides: Promising Catalysts or False Positives?

Izelaar, B. (author), Ripepi, D. (author), Asperti, S. (author), Dugulan, A.I. (author), Hendrikx, R.W.A. (author), Bottger, A.J. (author), Mulder, F.M. (author), Kortlever, R. (author)

The electrochemical dinitrogen reduction reaction (NRR) has recently gained much interest as it can potentially produce ammonia from renewable intermittent electricity and replace the Haber-Bosch process. Previous literature studies report Fe- and Mo-carbides as promising electrocatalysts for the NRR with activities higher than other metals....

journal article 2023

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Unravelling the Effect of Activators used in The Synthesis of Biomass-Derived Carbon Electrocatalysts on the Electrocatalytic Performance for CO₂ Reduction

Fu, S. (author), Li, M. (author), Asperti, S. (author), de Jong, W. (author), Kortlever, R. (author)

N-doped carbon materials can be efficient and cost-effective catalysts for the electrochemical CO₂ reduction reaction (CO₂RR). Activators are often used in the synthesis process to increase the specific surface area and porosity of these carbon materials. However, owing to the diversity of activators and the differences...

journal article 2023

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Design of an elevated pressure electrochemical flow cell for CO₂ reduction

Morrison, A.R.T. (author), Girichandran, N. (author), Wols, Quincy (author), Kortlever, R. (author)

Abstract: The electrochemical CO₂ reduction reaction (CO₂RR) has been proposed as a sustainable way of closing the carbon cycle while synthesizing useful commodity chemicals. One of the possible routes to scale up the process is the elevated pressure CO₂RR, as this increases the concentration of the poorly...

journal article 2023

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Electrochemical CO₂ Reduction on Copper in Propylene Carbonate: Influence of Water Content and Temperature on the Product Distribution

Burgers, I.A.E. (author), Pérez-Gallent, Elena (author), Goetheer, Earl (author), Kortlever, R. (author)

Aqueous electrolytes are most commonly used for the CO₂ reduction reaction (CO₂RR), but suffer from a low CO₂ solubility that limits the reaction. Electrochemical CO₂ reduction in nonaqueous electrolytes can provide a solution, due to the higher CO₂ solubility of organic solvent-based...

journal article 2023

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Tuning the Properties of N-Doped Biochar for Selective CO₂ Electroreduction to CO

Fu, S. (author), Li, M. (author), de Jong, W. (author), Kortlever, R. (author)

Nitrogen-doped (N-doped) carbon catalysts have been widely studied for electrochemical CO₂ reduction to CO. However, the correlation between the physicochemical properties of N-doped carbon catalysts and their electrocatalytic performance for the CO₂RR is still unclear. Herein, a series of N-doped biochar catalysts with...

journal article 2023

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Electrochemical cell design and performance evaluation of polyvinyl ferrocene/carbon nanotube electrodes for selective formate separation

Polat, S. (author), Kortlever, R. (author), Eral, H.B. (author)

Selective ion separation is a fundamental challenge with applications ranging from the manufacturing of pharmaceuticals & industrial salts to water desalination. In particular, the separation of formate, a primary product of electrochemical carbon dioxide reduction, has attracted attention not only to reduce carbon emissions and energy...

journal article 2023

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Towards Higher NH₃ Faradaic Efficiency: Selective-Poisoning of HER Active Sites by Co-Feeding CO in NO Electroreduction**

Li, M. (author), Verkuil, Jarco (author), Bunea, S. (author), Kortlever, R. (author), Urakawa, A. (author)

Direct electroreduction of nitric oxide offers a promising avenue to produce valuable chemicals, such as ammonia, which is an essential chemical to produce fertilizers. Direct ammonia synthesis from NO in a polymer electrolyte membrane (PEM) electrolyzer is advantageous for its continuous operation and excellent mass transport characteristics...

journal article 2023

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Identification, Quantification, and Elimination of NO_x and NH₃ Impurities for Aqueous and Li-Mediated Nitrogen Reduction Experiments

Izelaar, B. (author), Ripepi, D. (author), van Noordenne, D.D. (author), Jungbacker, M.P. (author), Kortlever, R. (author), Mulder, F.M. (author)

journal article 2023

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Benchmarking the Electrochemical CO₂ Reduction on Polycrystalline Copper Foils: The Importance of Microstructure Versus Applied Potential

Asperti, S. (author), Hendrikx, R.W.A. (author), Gonzalez Garcia, Y. (author), Kortlever, R. (author)

Copper is one of the most promising catalysts for the CO₂ reduction reaction (CO₂RR) due to its unique capability of producing multicarbon products in appreciable quantities. Most of the CO₂RR research efforts have been directed towards the development of new electrocatalysts to either increase product...

journal article 2022

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Surface Coverage as an Important Parameter for Predicting Selectivity Trends in Electrochemical CO₂ Reduction

Morrison, A.R.T. (author), Ramdin, M. (author), van den Broeke, L.J.P. (author), de Jong, W. (author), Vlugt, T.J.H. (author), Kortlever, R. (author)

The electrochemical CO2 reduction reaction (CO2RR) is important for a sustainable future. Key insights into the reaction pathways have been obtained by density functional theory (DFT) analysis, but so far, DFT has been unable to give an overall understanding of selectivity trends without important caveats. We show that an unconsidered...

journal article 2022

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Electrochemical Reduction of CO₂to Oxalic Acid: Experiments, Process Modeling, and Economics

Boor, Vera (author), Frijns, Jeannine E.B.M. (author), Laitinen, Antero T. (author), Goetheer, E.L.V. (author), van den Broeke, L.J.P. (author), Kortlever, R. (author), de Jong, W. (author), Moultos, O. (author), Vlugt, T.J.H. (author), Ramdin, M. (author)

We performed H-cell and flow cell experiments to study the electrochemical reduction of CO2 to oxalic acid (OA) on a lead (Pb) cathode in various nonaqueous solvents. The effects of anolyte, catholyte, supporting electrolyte, temperature, water content, and cathode potential on the Faraday efficiency (FE), current density (CD), and product...

journal article 2022

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Ultrasound-promoted preparation of polyvinyl ferrocene-based electrodes for selective formate separation: Experimental design and optimization

Polat, S. (author), Kortlever, R. (author), Eral, H.B. (author)

The selective separation of ions is a major technological challenge having far-ranging impacts from product separation in electrochemical production of base chemicals from CO₂ to water purification. In recent years, ion-selective electrochemical systems leveraging redox-materials emerged as an attractive platform based on their...

journal article 2022

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Nanostructuring Pt-Pd Bimetallic Electrocatalysts for CO₂ Reduction Using Atmospheric Pressure Atomic Layer Deposition

Li, M. (author), Fu, S. (author), Saedy, S. (author), Rajendrakumar, Aparna (author), Tichelaar, F.D. (author), Kortlever, R. (author), van Ommen, J.R. (author)

Preparing supported nanoparticles with a well-defined structure, uniform particle size, and composition using conventional catalyst synthesis methods, such as impregnation, precipitation, and deposition-precipitation is challenging. Furthermore, these liquid phase methods require significant solvent consumption, which has sustainable issues...

journal article 2022

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Effect of different alkali metal cations on the oxygen evolution activity and battery capacity of nickel electrodes in concentrated hydroxide electrolytes

Mangel Raventos, A. (author), Kortlever, R. (author)

The effect of different alkali metal cations on the oxygen evolution activity and battery capacity of nickel electrodes has recently been studied in low concentration alkali hydroxide electrolytes. As high concentration hydroxide electrolytes are favored in applications due to their high conductivity, we investigate if the cation effects...

journal article 2022

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Electroreduction of CO₂/CO to C₂Products: Process Modeling, Downstream Separation, System Integration, and Economic Analysis

Ramdin, M. (author), De Mot, Bert (author), Morrison, A.R.T. (author), Breugelmans, Tom (author), van den Broeke, L.J.P. (author), Kortlever, R. (author), de Jong, W. (author), Moultos, O. (author), Vlugt, T.J.H. (author)

Direct electrochemical reduction of CO2 to C2 products such as ethylene is more efficient in alkaline media, but it suffers from parasitic loss of reactants due to (bi)carbonate formation. A two-step process where the CO2 is first electrochemically reduced to CO and subsequently converted to desired C2 products has the potential to overcome...

journal article 2021

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Sn-Based Electrocatalyst Stability: A Crucial Piece to the Puzzle for the Electrochemical CO₂Reduction toward Formic Acid

Van Daele, Kevin (author), De Mot, Bert (author), Moura de Salles Pupo, M. (author), Daems, Nick (author), Pant, Deepak (author), Kortlever, R. (author), Breugelmans, Tom (author)

Nowadays, Sn-based electrocatalysts for the electrochemical CO2 reduction reaction (eCO2RR) toward formic acid have been reported to reach industrially relevant current densities and Faradaic efficiencies approaching 100%. However, electrocatalyst stability remains inadequate and appears to be a crucial piece to the puzzle, as lifetimes in...

journal article 2021

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Modeling the Performance of an Integrated Battery and Electrolyzer System

Mangel Raventos, A. (author), Kluivers, Gerard J. (author), Haverkort, J.W. (author), de Jong, W. (author), Mulder, F.M. (author), Kortlever, R. (author)

Both daily and seasonal fluctuations of renewable power sources will require large-scale energy storage technologies. A recently developed integrated battery and electrolyzer system, called battolyser, fulfills both time-scale requirements. Here, we develop a macroscopic COMSOL Multiphysics model to quantify the energetic efficiency of the...

journal article 2021

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Electrochemical CO₂ reduction on nanostructured metal electrodes: Fact or defect?

Kas, R. (author), Yang, K. (author), Bohra, D. (author), Kortlever, R. (author), Burdyny, T.E. (author), Smith, W.A. (author)

Electrochemical CO₂ reduction has received an increased amount of interest in the last decade as a promising avenue for storing renewable electricity in chemical bonds. Despite considerable progress on catalyst performance using nanostructured electrodes, the sensitivity of the reaction to process conditions has led to debate on...

review 2020

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In Situ ATR-SEIRAS of Carbon Dioxide Reduction at a Plasmonic Silver Cathode

Corson, Elizabeth R. (author), Kas, R. (author), Kostecki, Robert (author), Urban, Jeffrey J. (author), Smith, W.A. (author), McCloskey, Bryan D. (author), Kortlever, R. (author)

Illumination of a voltage-biased plasmonic Ag cathode during CO2 reduction results in a suppression of the H2 evolution reaction while enhancing CO2 reduction. This effect has been shown to be photonic rather than thermal, but the exact plasmonic mechanism is unknown. Here, we conduct an in situ ATR-SEIRAS (attenuated total reflectance...

journal article 2020