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Kolen, M. (author), Smith, W.A. (author), Mulder, F.M. (author)Direct electrolytic N2 reduction to ammonia (NH3) is a renewable alternative to the Haber-Bosch process. The activity and selectivity of electrocatalysts are evaluated by measuring the amount of NH3 in the electrolyte. Quantitative 1H nuclear magnetic resonance (qNMR) detection reduces the bench time to analyze samples of NH3 (present in the...journal article 2021
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Kas, Recep (author), Star, Andrew G. (author), Yang, K. (author), Van Cleve, Tim (author), Neyerlin, Kenneth C. (author), Smith, W.A. (author)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...journal article 2021
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Yang, K. (author), Kas, Recep (author), Smith, W.A. (author), Burdyny, T.E. (author)The deployment of gas diffusion electrodes (GDEs) for the electrochemical CO2 reduction reaction (CO2RR) has enabled current densities an order of magnitude greater than those of aqueous H cells. The gains in production, however, have come with stability challenges due to rapid flooding of GDEs, which frustrate both laboratory experiments and...journal article 2021
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Bae, D. (author), Kanellos, Gerasimos (author), Faasse, G.M. (author), Dražević, Emil (author), Venugopal, A. (author), Smith, W.A. (author)Recent advances in photoelectrochemical redox flow cells, such as solar redox flow batteries, have received much attention as an alternative integrated technology for simultaneous conversion and storage of solar energy. Theoretically, it has been reported that even single- photon devices can demonstrate unbiased photo-charging with high solar-to...journal article 2020
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Bae, D. (author), Faasse, Richard (author), Smith, W.A. (author)Achieving high current densities without thermal performance degradation at high temperatures is one of the main challenges for enhancing the competitiveness of photo-electrochemical energy storage systems. We describe a system that overcomes this challenge by incorporating an integrated photoelectrode with a redox flow cell, which functions...journal article 2020
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Nesbitt, Nathan T. (author), Burdyny, T.E. (author), Salvatore, Danielle (author), Bohra, D. (author), Kas, Recep (author), Smith, W.A. (author)Electrochemical CO2 electrolysis to produce hydrocarbon fuels or material feedstocks offers a renewable alternative to fossilized carbon sources. Gas-diffusion electrodes (GDEs), composed of solid electrocatalysts on porous supports positioned near the interface of a conducting electrolyte and CO2 gas, have been able to demonstrate the...journal article 2020
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Vos, Johannes G. (author), Venugopal, A. (author), Smith, W.A. (author), Koper, Marc T.M. (author)Hydrogen production from seawater electrolysis is highly promising for the capture and storage of intermittent renewable energy, but is hindered by the possibility of unwanted reactions at the anode. The oxidation reactions of chloride and (to a lesser extent) bromide, which can occur in parallel to the evolution of oxygen, lead to...journal article 2020
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Kas, R. (author), Yang, K. (author), Bohra, D. (author), Kortlever, R. (author), Burdyny, T.E. (author), Smith, W.A. (author)Electrochemical CO<sub>2</sub> 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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Bae, D. (author), Kanellos, Gerasimos (author), Wedege, Kristina (author), Dražević, Emil (author), Bentien, Anders (author), Smith, W.A. (author)MoOX is commonly considered to be a high work-function semiconductor. From x-ray photoelectron spectroscopy and photoelectrochemical analysis, it is shown that MoOX can be considered as an effective hole transfer layer for the GaP-based device. Specifically, in the absence of carbon contamination using an ion beam cleaning step, the oxygen...journal article 2020
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Vos, Johannes G. (author), Venugopal, A. (author), Smith, W.A. (author), Koper, Marc T.M. (author)During hydrogen production for (renewable) energy storage, direct seawater electrolysis offers several notable advantages over freshwater electrolysis. Unfortunately, it is also hindered by possible oxidation reactions of chloride and (to a lesser extent) bromide, which can occur in parallel to the evolution of oxygen and form harmful by...journal article 2020
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De Gregorio, Gian Luca (author), Burdyny, T.E. (author), Loiudice, Anna (author), Iyengar, Pranit (author), Smith, W.A. (author), Buonsanti, Raffaella (author)Despite substantial progress in the electrochemical conversion of CO<sub>2</sub> into value-added chemicals, the translation of fundamental studies into commercially relevant conditions requires additional efforts. Here, we study the catalytic properties of tailored Cu nanocatalysts under commercially relevant current densities in a gas-fed...journal article 2020
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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
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Blommaert, M.A. (author), Verdonk, J.A.H. (author), Blommaert, Hester C.B. (author), Smith, W.A. (author), Vermaas, D.A. (author)A bipolar membrane (BPM) can be used to accelerate water dissociation to maintain a pH gradient in electrochemical cells, providing freedom to independently optimize the environments and catalysts used for paired reduction and oxidation reactions. The two physical layers in a BPM, respectively, selective for the exchange of cations and anions...journal article 2020
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- Liu, K. (author), Smith, W.A. (author), Burdyny, Thomas (author) review 2019
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Bohra, D. (author), Chaudhry, Jehanzeb H. (author), Burdyny, T.E. (author), Pidko, E.A. (author), Smith, W.A. (author)The environment of a CO2 electroreduction (CO2ER) catalyst is intimately coupled with the surface reaction energetics and is therefore a critical aspect of the overall system performance. The immediate reaction environment of the electrocatalyst constitutes the electrical double layer (EDL) which extends a few nanometers into the electrolyte and...journal article 2019
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Burdyny, T.E. (author), Smith, W.A. (author)Electrocatalytic CO <sub>2</sub> reduction has the dual-promise of neutralizing carbon emissions in the near future, while providing a long-term pathway to create energy-dense chemicals and fuels from atmospheric CO <sub>2</sub> . The field has advanced immensely in recent years, taking significant strides towards commercial realization....journal article 2019
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Liu, K. (author), Ma, M. (author), Wu, Longfei (author), Valenti, M. (author), Cardenas-Morcoso, Drialys (author), Hofmann, Jan P. (author), Bisquert, Juan (author), Gimenez, Sixto (author), Smith, W.A. (author)Au-Cu bimetallic thin films with controlled composition were fabricated by magnetron sputtering co-deposition, and their performance for the electrocatalytic reduction of CO <sub>2</sub> was investigated. The uniform planar morphology served as a platform to evaluate the electronic effect isolated from morphological effects while minimizing...journal article 2019
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Bae, D. (author), Faasse, Richard (author), Kanellos, Gerasimos (author), Smith, W.A. (author)In recent years, solar redox flow batteries have attracted attention as a possible integrated technology for simultaneous conversion and storage of solar energy. Unlike solar water splitting technologies which require at least 1.8V for meaningful performance, a lesson learned from previous solar redox flow battery (SRFB) studies is that even...journal article 2019
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Yang, K. (author), Kas, R. (author), Smith, W.A. (author)Over the past decade, electrochemical carbon dioxide reduction has become a thriving area of research with the aim of converting electricity to renewable chemicals and fuels. Recent advances through catalyst development have significantly improved selectivity and activity. However, drawing potential dependent structure-activity relationships...journal article 2019
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Bohra, D. (author), Ledezma Yanez, I.D. (author), Li, G. (author), de Jong, W. (author), Pidko, E.A. (author), Smith, W.A. (author)Ag is a promising catalyst for the production of carbon monoxide (CO) via the electrochemical reduction of carbon dioxide (CO<sub>2</sub>ER). Herein, we study the role of the formate (HCOO<sup>−</sup>) intermediate *OCHO, aiming to resolve the discrepancy between the theoretical understanding and experimental performance of Ag. We show that...journal article 2019