Searched for: author%3A%22Smith%2C+W.A.%22
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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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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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Ripepi, D. (author), Izelaar, B. (author), van Noordenne, D.D. (author), Jungbacker, M.P. (author), Kolen, M. (author), Karanth, P. (author), Cruz, Daniel (author), Zeller, Patrick (author), Pérez-Dieste, Virginia (author), Villar-Garcia, Ignacio J. (author), Smith, W.A. (author), Mulder, F.M. (author)
Hydrogen permeable electrodes can be utilized for electrolytic ammonia synthesis from dinitrogen, water, and renewable electricity under ambient conditions, providing a promising route toward sustainable ammonia. The understanding of the interactions of adsorbing N and permeating H at the catalytic interface is a critical step toward the...
journal article 2022
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Kolen, M. (author), Antoniadis, Grigorios (author), Schreuders, H. (author), Boshuizen, B. (author), van Noordenne, D.D. (author), Ripepi, D. (author), Smith, W.A. (author), Mulder, F.M. (author)
The electrochemical nitrogen reduction reaction (NRR) is a promising alternative to the current greenhouse gas emission intensive process to produce ammonia (NH<sub>3</sub>) from nitrogen (N<sub>2</sub>). However, finding an electrocatalyst that promotes NRR over the competing hydrogen evolution reaction (HER) has proven to be difficult. This...
journal article 2022
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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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Brimley, Paige (author), Almajed, Hussain (author), Alsunni, Yousef (author), Alherz, Abdulaziz W. (author), Bare, Zachary J.L. (author), Smith, W.A. (author), Musgrave, Charles B. (author)
Renewably driven, electrochemical conversion of carbon dioxide into value-added products is expected to be a critical tool in global decarbonization. However, theoretical studies based on the computational hydrogen electrode largely ignore the nonlinear effects of the applied potential on the calculated results, leading to inaccurate...
journal article 2022
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Kas, Recep (author), Yang, K. (author), Yewale, Gaurav P. (author), Crow, Allison (author), Burdyny, T.E. (author), Smith, W.A. (author)
The electrochemical reduction of bicarbonate to renewable chemicals without external gaseous CO2 supply has been motivated as a means of integrating conversion with upstream CO2 capture. The way that CO2 is formed and transported during CO2-mediated bicarbonate reduction in flow cells is profoundly different from conventional CO2 saturated...
journal article 2022
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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...
review 2022
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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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Batista, Victor (author), Li, Can (author), Smith, W.A. (author), Wang, Dunwei (author)
contribution to periodical 2021
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Chandrashekar, S. (author), Geerlings, J.J.C. (author), Smith, W.A. (author)
The field of electrochemical CO<sub>2</sub> reduction has been transitioning to industrially relevant scales by changing the architecture of the electrochemical cells and moving away from the traditional aqueous H-cells to membrane electrode assemblies (MEA). The reaction environments in MEAs vary drastically from that of aqueous H-cells,...
journal article 2021
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Venugopal, A. (author), Kas, Recep (author), Hau, Kayeu (author), Smith, W.A. (author)
Detailed knowledge about the semiconductor/electrolyte interface in photoelectrochemical (PEC) systems has been lacking because of the inherent difficulty of studying such interfaces, especially during operation. Current understandings of these interfaces are mostly from the extrapolation of ex situ data or from modeling approaches. Hence,...
journal article 2021
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Yang, K. (author), Li, Mengran (author), Subramanian, S.S. (author), Blommaert, M.A. (author), Smith, W.A. (author), Burdyny, T.E. (author)
Advancing reaction rates for electrochemical CO2 reduction in membrane electrode assemblies (MEAs) have boosted the promise of the technology while exposing new shortcomings. Among these is the maximum utilization of CO2, which is capped at 50% (CO as targeted product) due to unwanted homogeneous reactions. Using bipolar membranes in an MEA ...
journal article 2021
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Blommaert, M.A. (author), Subramanian, S.S. (author), Yang, K. (author), Smith, W.A. (author), Vermaas, D.A. (author)
Typically, anion exchange membranes (AEMs) are used in CO2 electrolyzers, but those suffer from unwanted CO2 crossover, implying (indirect) energy consumption for generating an excess of CO2 feed and purification of the KOH anolyte. As an alternative, bipolar membranes (BPMs) have been suggested, which mitigate the reactant loss by...
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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Buonsanti, Raffaella (author), Smith, W.A. (author)
journal article 2021
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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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Blommaert, M.A. (author), sharifian, rezvan (author), Shah, N. (author), Nesbitt, N.T. (author), Smith, W.A. (author), Vermaas, D.A. (author)
A bipolar membrane (BPM), consisting of a cation and an anion exchange layer (CEL and AEL), can be used in an electrochemical cell in two orientations: reverse bias and forward bias. A reverse bias is traditionally used to facilitate water dissociation and control the pH at either side. A forward bias has been proposed for several...
journal article 2021
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Nesbitt, N.T. (author), Smith, W.A. (author)
Electrochemical atomic force microscopy (EC-AFM) enables measurement of electrode topography and mechanical properties during electrochemical reactions. However, for aqueous-based reactions that make gas products, such as CO2 reduction and water splitting into CO/H2, current densities below 1 mA cm-2 have been necessary to prevent formation...
journal article 2021
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