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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
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Firet, N.J. (author), Blommaert, M.A. (author), Burdyny, T.E. (author), Venugopal, A. (author), Bohra, D. (author), Longo, Alessandro (author), Smith, W.A. (author)Electrocatalysis of carbon dioxide can provide a valuable pathway towards the sustainable production of chemicals and fuels from renewable electricity sources. One of the main challenges to enable this technology is to find suitable electrodes that can act as efficient, stable and selective CO<sub>2</sub> reduction catalysts. Modified silver...journal article 2019
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Zhang, W. (author), Ma, M. (author), Huijbers, M.M.E. (author), Filonenko, G.A. (author), Pidko, E.A. (author), van Schie, M.M.C.H. (author), de Boer, Sabrina (author), Smith, W.A. (author), Hollmann, F. (author)A recently discovered photodecarboxylase from Chlorella variabilis NC64A ( CvFAP) bears the promise for the efficient and selective synthesis of hydrocarbons from carboxylic acids. CvFAP, however, exhibits a clear preference for long-chain fatty acids thereby limiting its broad applicability. In this contribution, we demonstrate that the...journal article 2019
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Perez Rodriguez, P. (author), Vijselaar, Wouter (author), Huskens, Jurriaan (author), Stam, Machiel (author), Falkenberg, M. (author), Zeman, M. (author), Smith, W.A. (author), Smets, A.H.M. (author)Solar fuels are a promising way to store solar energy seasonally. This paper proposes an earth-abundant heterostructure to split water using a photovoltaic-electrochemical device (PV-EC). The heterostructure is based on a hybrid architecture of a thin-film (TF) silicon tandem on top of a c-Si wafer (W) heterojunction solar cell (a-Si:H (TF)...journal article 2019
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Valenti, M. (author), Prasad, Nitin P. (author), Kas, R. (author), Bohra, D. (author), Ma, M. (author), Balasubramanian, Vignesh (author), Chu, L. (author), Dam, B. (author), Smith, W.A. (author)CO <sub>2</sub> electroreduction is a promising technology to produce chemicals and fuels from renewable resources. Polycrystalline and nanostructured metals have been tested extensively while less effort has been spent on understanding the performance of bimetallic alloys. In this work, we study compositionally variant, smooth Au-Pd thin...journal article 2019
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Smith, W.A. (author), Burdyny, T.E. (author), Vermaas, D.A. (author), Geerlings, J.J.C. (author)Using renewable energy as an input, Power-to-X technologies have the potential to replace fossil fuels and chemicals with dense-energy carriers that are instead derived out of thin air. In this work, we put into context what the industrial-scale production of chemicals from ambient CO<sub>2</sub> using CO<sub>2</sub> electrolysis means in...review 2019
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Firet, N.J. (author), Venugopal, A. (author), Blommaert, M.A. (author), Cavallari, Chiara (author), Sahle, Christoph J. (author), Longo, Alessandro (author), Smith, W.A. (author)Photocharging has recently been demonstrated as a powerful method to improve the photoelectrochemical water splitting performance of different metal oxide photoanodes, including BiVO<sub>4</sub>. In this work, we use ambient-pressure X-ray Raman scattering (XRS) spectroscopy to study the surface electronic structure of photocharged BiVO<sub>4...journal article 2019
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Kas, R. (author), Ayemoba, Onagie (author), Firet, N.J. (author), Middelkoop, J. (author), Smith, W.A. (author), Cuesta, Angel (author)The field of electrochemical CO<sub>2</sub> conversion is undergoing significant growth in terms of the number of publications and worldwide research groups involved. Despite improvements of the catalytic performance, the complex reaction mechanisms and solution chemistry of CO<sub>2</sub> have resulted in a considerable amount of...review 2019
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Wang, R. (author), Haspel, Henrik (author), Pustovarenko, Alexey (author), Dikhtiarenko, A. (author), Osadchii, D. (author), Ma, M. (author), Smith, W.A. (author), Kapteijn, F. (author), Gascon, Jorge (author)We report the preparation and electrocatalytic performance of silver-containing gas diffusion electrodes (GDEs) derived from a silver coordination polymer (Ag-CP). Layer-by-layer growth of the Ag-CP onto porous supports was applied to control Ag loading. Subsequent electro-decomposition of the Ag-CP resulted in highly selective and efficient...journal article 2019
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Blommaert, M.A. (author), Vermaas, D.A. (author), Izelaar, Boaz (author), In'T Veen, Ben (author), Smith, W.A. (author)A bipolar membrane (BPM) can be used to maintain a pH difference in an electrolysis cell, which provides freedom to independently optimize the environments and catalysts used for paired redox reactions. A BPM consists of two physical layers, of which one is selective for the exchange of cations and the other for anions. The water dissociation...journal article 2019
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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