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A better understanding of interfacial mechanisms is needed to improve the performances of electrochemical devices. Yet, simulating an electrode surface at fixed electrolyte composition remains a challenge. Here we apply a finite electric…

Materials Science · Physics 2019-11-13 Thomas Dufils , Guillaume Jeanmairet , Benjamin Rotenberg , Michiel Sprik , Mathieu Salanne

While fluids near a solid surface are at the core of applications in energy storage/conversion, electrochemistry/electrowetting and adsorption/catalysis, their nanoscale behavior remains only partially deciphered. Beyond conventional…

Soft Condensed Matter · Physics 2026-01-07 Cecilia Herrero , Lyderic Bocquet , Benoit Coasne

Electrochemical CO2 reduction offers a method to use renewable electricity to convert CO2 into CO and other carbon-based chemical building blocks. While nearly all studies rely on a CO2 feed, we show herein that aqueous bicarbonate…

In this work, we examine metal electrode-ionomer electrolyte systems at high voltage / negative surface charge and at high pH to assess factors that influence hydrogen production efficiency. We simulate the hydrogen evolution electrode…

Chemical Physics · Physics 2019-09-04 Reese E. Jones , William C. Tucker , Matthew J. L. Mills , Sanjeev Mukerjee

We explore the force generation and surface interactions arising when electric fields are applied across fluid films. Using a surface force balance (SFB) we measure directly the force between two electrodes in crossed-cylinder geometry…

Soft Condensed Matter · Physics 2019-04-09 Carla Perez-Martinez , Susan Perkin

Understanding the evolution of electrified solid-liquid interfaces during electrochemical reactions is crucial. However, capturing the dynamic behavior of the interfaces with high temporal resolution and accuracy over long timescales…

Chemical Physics · Physics 2024-11-26 Letian Chen , Yun Tian , Xu Hu , Suya Chen , Huijuan Wang , Xu Zhang , Zhen Zhou

Electric fields have been highlighted as a smart reagent in nature's enzymatic machinery, as they can directly trigger or accelerate redox and/or non-redox chemical processes with stereo- and regio-specificity. In natural catalysis,…

The response of water to electric fields is critical to the performance and stability of electrochemical devices, and the selectivity of enzymatic, atmospheric, and organic reactions. A key process in this context is the water…

Chemical Physics · Physics 2025-10-10 Yair Litman , Angelos Michaelides

A general physics-based model is developed for heterogeneous electrocatalysis in porous electrodes and used to predict and interpret the impedance of solid oxide fuel cells. This model describes the coupled processes of oxygen gas…

Chemical Physics · Physics 2014-12-05 Y. Fu , S. Poizeau , A. Bertei , C. Qi , A. Mohanram , J. D. Pietras , M. Z. Bazant

A major challenge in modelling interfacial processes in electrochemical (EC) devices is performing simulations at constant potential. This requires an open-boundary description of the electrons, so that they can enter and leave the…

Chemical Physics · Physics 2023-11-07 Margherita Buraschi , Andrew P. Horsfield , Clotilde S. Cucinotta

Electrochemical interfaces are of fundamental importance in electrocatalysis, batteries, and metal corrosion. Finite-field methods are one of most reliable approaches for modeling electrochemical interfaces in complete cells under realistic…

Chemical Physics · Physics 2025-06-13 Chaoqiang Feng , Bin Jiang

A comprehensive understanding of the electrode-electrolyte interface in energy conversion systems remains challenging due to the complex and multifaceted nature of interfacial processes. This complexity hinders the development of more…

Chemical Physics · Physics 2024-10-23 Ben Wang , Tomohiro Fukushima , Hiro Minamimoto , Andrey Lyalin , Kei Murakoshi , Tetsuya Taketsugu

Ionic liquids are widely used as electrolytes in electrochemical devices. In this context, many experimental and theoretical approaches have been recently developed for characterizing their interface with electrodes. In this perspective…

Materials Science · Physics 2017-09-13 Céline Merlet , Benjamin Rotenberg , Paul Madden , Mathieu Salanne

The electrical double layer (EDL) at aqueous solution-metal oxide interfaces critically affects many fundamental processes in electrochemistry, geology and biology, yet understanding its microscopic structure is challenging for both theory…

Two of the most challenging tasks in molecular simulation consist in capturing the properties of systems with long-range interactions (e.g. electrolyte solutions) as well as systems containing large molecules such as hydrogels. For the…

Chemical Physics · Physics 2011-07-26 Jonathan Walter , Stephan Deublein , Steffen Reiser , Martin Horsch , Jadran Vrabec , Hans Hasse

The results of molecular dynamics simulations of the properties of water in an aqueous ionic solution close to an interface with a model metallic electrode are described. In the simulations the electrode behaves as an ideally polarizable…

Statistical Mechanics · Physics 2014-09-09 Adam P. Willard , Stewart K. Reed , Paul A. Madden , David Chandler

Many key industrial processes, from electricity production, conversion and storage to electrocatalysis or electrochemistry in general, rely on physical mechanisms occurring at the interface between a metallic electrode and an electrolyte…

Computational Physics · Physics 2021-09-03 Laura Scalfi , Mathieu Salanne , Benjamin Rotenberg

Electro-osmosis (EO) is a powerful tool to manipulate liquids in micro and nanofluidic systems. While EO has been studied extensively at liquid-solid interfaces, the case of liquid-vapor interfaces, found e.g. in foam films and bubbles,…

Soft Condensed Matter · Physics 2021-11-23 Alexia Barbosa de Lima , Laurent Joly

We apply first principles computational techniques to analyze the two-electron, multi-step, electrochemical reduction of CO2 to CO in water using cobalt porphyrin as a catalyst. Density Functional Theory calculations with hybrid functionals…

Chemical Physics · Physics 2011-01-06 Kevin Leung , Ida M. B. Nielsen , Na Sai , Craig J. Medforth , J. A. Shelnutt

High electric fields can significantly alter catalytic environments and the resultant chemical processes. Such fields arise naturally in biological systems but can also be artificially induced through localized excitations at nanoscale.…

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