Journal ArticleDOI
Along the Channel Gradients Impact on the Spatioactivity of Gas Diffusion Electrodes at High Conversions during CO2 Electroreduction
Recep Kas,Recep Kas,Andrew G. Star,Kailun Yang,Tim Van Cleve,Kenneth C. Neyerlin,Wilson A. Smith +6 more
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TLDR
In this paper, a 2D transport model for a gas diffusion electrode performing CO₂ reduction to CO with a flowing catholyte is presented, including the concentration gradients along the flow cell, spatial distribution of the current density and local pH in the catalyst layer.Abstract:
Results of a 2-D transport model for a gas diffusion electrode performing CO₂ reduction to CO with a flowing catholyte are presented, including the concentration gradients along the flow cell, spatial distribution of the current density and local pH in the catalyst layer. The model predicts that both the concentration of CO₂ and the buffer electrolyte gradually diminish along the channels for a parallel flow of gas and electrolyte as a result of electrochemical conversion and nonelectrochemical consumption. At high single-pass conversions, significant concentration gradients exist along the flow channels leading to large local variations in the current density (>150 mA/cm²), which becomes prominent when compared to ohmic losses. In addition, concentration overpotentials change dramatically with CO₂ flow rate, which results in significant differences in outlet concentrations at high conversions. The outlet concentration of CO attains a maximum of 80% along with 5% CO₂ and 15% H₂, although the maximum single-pass conversion is limited to below 60% due to homogeneous consumption by the electrolyte. Fundamental and practical implications of our findings on electrochemical CO₂ reduction are discussed with a focus on the trade-off between high current density operation and high single-pass conversion efficiency.read more
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Journal ArticleDOI
Highly selective and productive reduction of carbon dioxide to multicarbon products via in situ CO management using segmented tandem electrodes
TL;DR: In this paper , a segmented gas-diffusion electrode (s-GDE) was designed to prolong the residence time of CO (produced by the first catalyst) at the second catalyst, resulting in high production of further reduced yields.
Journal ArticleDOI
Cation-Driven Increases of CO2 Utilization in a Bipolar Membrane Electrode Assembly for CO2 Electrolysis
Kailun Yang,Mengran Li,Siddhartha Subramanian,Marijn A. Blommaert,Wilson A. Smith,Thomas Burdyny +5 more
Journal ArticleDOI
Process modeling, techno-economic assessment, and life cycle assessment of the electrochemical reduction of CO2: a review.
Ana Somoza-Tornos,Omar J. Guerra,Allison M. Crow,Allison M. Crow,Wilson A. Smith,Wilson A. Smith,Bri-Mathias Hodge,Bri-Mathias Hodge +7 more
TL;DR: In this article, the authors provide a comprehensive overview of techno-economic and life cycle assessment methods and pave the way for future assessment approaches, and assess the challenges and research opportunities for the industrial implementation of CO2 reduction via electrolysis.
Journal ArticleDOI
Modeling Operando Electrochemical CO2 Reduction.
TL;DR: In this article , the potential of density functional theory and machine learning to interpret data from Operando spectroelectrochemical techniques, such as Raman spectroscopy and extended X-ray absorption fine structure characterization, is discussed.
References
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Journal ArticleDOI
Status and perspectives of CO2 conversion into fuels and chemicals by catalytic, photocatalytic and electrocatalytic processes
Evgenii V. Kondratenko,Guido Mul,Jonas Baltrusaitis,Gastón O. Larrazábal,Javier Pérez-Ramírez +4 more
TL;DR: In this paper, a review of recent developments and future perspectives in carbon dioxide usage for sustainable production of energy and chemicals and to reduce global warming is presented, focusing on the design of metal electrodes to improve their performance and recent developments of alternative approaches such as the application of ionic liquids as electrolytes and microorganisms as co-catalysts.
Journal ArticleDOI
CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
Cao-Thang Dinh,Thomas Burdyny,Golam Kibria,Ali Seifitokaldani,Christine M. Gabardo,F. Pelayo García de Arquer,Amirreza Kiani,Jonathan P. Edwards,Phil De Luna,Oleksandr S. Bushuyev,Chengqin Zou,Chengqin Zou,Rafael Quintero-Bermudez,Yuanjie Pang,David Sinton,Edward H. Sargent +15 more
TL;DR: A copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO2 to ethylene with 70% faradaic efficiency at a potential of −0.55 volts versus a reversible hydrogen electrode (RHE).
Journal ArticleDOI
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
Yuvraj Y. Birdja,Yuvraj Y. Birdja,Elena Pérez-Gallent,Marta C. Figueiredo,Marta C. Figueiredo,Adrien J. Göttle,Federico Calle-Vallejo,Federico Calle-Vallejo,Marc T. M. Koper +8 more
TL;DR: In this article, the authors review recent advances and challenges in the understanding of electrochemical CO2 reduction and discuss existing models for the initial activation of CO2 on the electrocatalyst and their importance for understanding selectivity.
Journal ArticleDOI
Thin-film catalyst layers for polymer electrolyte fuel cell electrodes
TL;DR: In this paper, the Pt/C catalyst layer of polymer electrolyte fuel cell electrodes have been developed that substantially increase the utilization efficiency of the catalyst, and the performance of fuel cells based on the thin film catalyst layers are comparable with those of gas diffusion electrode designs that utilize several times as much platinum, thus the specific catalysts in the new structures are significantly higher.
Journal ArticleDOI
General Techno-Economic Analysis of CO2 Electrolysis Systems
TL;DR: In this article, the authors present an economic analysis to calculate the end-of-life net present value (NPV) of a generalized CO2 electrolyzer system for the production of 100 tons/day of various CO2 reduction products.
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