document

Solar fuel production by using PV/PEC junctions based on earth-abundant materials

Perez Rodriguez, P. (author), Digdaya, I.A. (author), Mangel Raventos, A. (author), Falkenberg, M. (author), Vasudevan, R.A. (author), Zeman, M. (author), Smith, W.A. (author), Smets, A.H.M. (author)

One of the main problems of renewable energies is storage of the energy carrier. For long-term storage, solar fuels seem to be a good option. Direct solar water splitting could play an important role in the production of these solar fuels. One of the main challenges of this process is the charge separation and collection at the interfaces. The...

conference paper 2016

document

Introducing special issue on photocatalysis and photoelectrochemistry

Batista, Victor (author), Li, Can (author), Smith, W.A. (author), Wang, Dunwei (author)

contribution to periodical 2021

document

Investigation of Terahertz Emission from BiVO4 /Au Thin Film Interface

Kumar, N. (author), Abdi, F.F. (author), Trzesniewski, B. (author), Smith, W.A. (author), Planken, P.C.M. (author), Adam, A.J.L. (author)

We demonstrate emission of terahertz pulses from a BiVO4/Au thin film interface, illuminated with femtosecond laser pulses. Based on the experimental observations, we propose that the most likely cause of the THz emission is the Photo-Dember effect caused by the standing wave intensity distribution formed at the BiVO4/Au interfaces.

journal article 2015

document

Photocharged BiVO4 photoanodes for improved solar water splitting

Trze?niewski, B.J. (author), Smith, W.A. (author)

Bismuth vanadate (BiVO4) is a promising semiconductor material for the production of solar fuels via photoelectrochemical water splitting, however, it suffers from substantial recombination losses that limit its performance to well below its theoretical maximum. Here we demonstrate for the first time that the photoelectrochemical (PEC)...

journal article 2015

document

Photo-assisted water splitting with bipolar membrane induced pH gradients for practical solar fuel devices

Vermaas, D.A. (author), Sassenburg, M. (author), Smith, W.A. (author)

Different pH requirements for a cathode and an anode result in a non-optimal performance for practical solar fuel systems. We present for the first time a photo-assisted water splitting device using a bipolar membrane, which allows a cathode to operate in an acidic electrolyte while the photoanode is in alkaline conditions. The bipolar membrane...

journal article 2015

document

Characterizing CO2 Reduction Catalysts on Gas Diffusion Electrodes: Comparing Activity, Selectivity, and Stability of Transition Metal Catalysts

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

document

Modeling the electrical double layer to understand the reaction environment in a CO2 electrocatalytic system

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

document

Design principles for efficient photoelectrodes in solar rechargeable redox flow cell applications

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

document

Hidden Figures of Photo-charging: a thermo-electrochemical approach for a solar-rechargeable redox flow cell system

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

document

Operando Topography and Mechanical Property Mapping of CO₂Reduction Gas-Diffusion Electrodes Operating at High Current Densities

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

document

Emerging collaborations at the forefront of growth in electrochemical synthesis

Buonsanti, Raffaella (author), Smith, W.A. (author)

journal article 2021

document

Evaluating the techno-economic potential of defossilized air-to-syngas pathways

Almajed, Hussain M. (author), Guerra, Omar J. (author), Smith, W.A. (author), Hodge, Bri Mathias (author), Somoza Tornos, A. (author)

Defossilizing the chemical industry using air-to-chemical processes offers a promising solution to driving down the emission trajectory to net-zero by 2050. Syngas is a key intermediate in the chemical industry, which can be produced from electrolytic H2 and air-sourced CO2. To techno-economically assess possible emerging air-to-syngas routes,...

journal article 2023

document

Liquid-Solid Boundaries Dominate Activity of CO₂Reduction on Gas-Diffusion Electrodes

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

document

Assessing Silver Palladium Alloys for Electrochemical CO₂ Reduction in Membrane Electrode Assemblies

Chandrashekar, S. (author), Geerlings, J.J.C. (author), Smith, W.A. (author)

The field of electrochemical CO₂ 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

document

High Indirect Energy Consumption in AEM-Based CO₂Electrolyzers Demonstrates the Potential of Bipolar Membranes

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

document

Orientation of a bipolar membrane determines the dominant ion and carbonic species transport in membrane electrode assemblies for CO₂reduction

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

document

Cation-Driven Increases of CO₂Utilization in a Bipolar Membrane Electrode Assembly for CO₂Electrolysis

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

document

Operando Infrared Spectroscopy Reveals the Dynamic Nature of Semiconductor-Electrolyte Interface in Multinary Metal Oxide Photoelectrodes

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

document

Investigating the role of potassium cations during electrochemical CO₂ reduction

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

document

Accelerating ¹H NMR Detection of Aqueous Ammonia

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