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Recent advances in calculating potential of zero charge and Helmholtz capacitance of metal/aqueous solution interfaces from ab initio molecular dynamics

CURRENT OPINION IN ELECTROCHEMISTRY (2023)

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Article Chemistry, Physical

Comparing Ab Initio Molecular Dynamics and a Semiclassical Grand Canonical Scheme for the Electric Double Layer of the Pt(111)/Water Interface

Jun Huang et al.

Summary: The theoretical modeling of metal/water interfaces focuses on the configuration of the electric double layer (EDL) under grand canonical conditions. Ab initio molecular dynamics (AIMD) simulations are ideal for treating water-metal interactions but are limited by small ensembles and short simulation times. Semiclassical approaches can efficiently handle the EDL model by averaging microscopic details. By combining AIMD and semiclassical methods, an improved description of the EDL can be obtained. Comparing these approaches using the Pt(111)/water interface, we analyze the differences in electric field, water configuration, and double-layer capacitance, and discuss their contributions to EDL theory.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2023)

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Article Chemistry, Physical

Machine Learning Assisted Simulations of Electrochemical Interfaces: Recent Progress and Challenges

Yipeng Zhou et al.

Summary: This Perspective article summarizes the recent progress and achievements in simulating electrochemical interfaces using machine learning. It discusses the limitations of current machine learning models, such as accurately describing long-range electrostatic interactions and the kinetics of electrochemical reactions at the interface. Finally, it points out future directions for machine learning to expand in the field of electrochemical interfaces.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2023)

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Article Chemistry, Physical

Optical method for quantifying the potential of zero charge at the platinum-water electrochemical interface

Pengtao Xu et al.

Summary: When an electrode contacts an electrolyte, an interfacial electric field forms. This field can be polarized by the electrode and nearby molecules, but this polarization can be neutralized by an applied potential. A new optical method is presented here to determine the potential of zero charge (pzc) at an electrochemical interface. The pzc of a Pt-water interface is found to be 0.23 +/- 0.08 V versus standard hydrogen electrode (SHE) and is pH independent. This research provides insights into the interfacial electrical field and water orientation without the need for probe molecules and confirms the intensity of the electric field during hydrogen electrocatalysis in alkaline conditions.

NATURE MATERIALS (2023)

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Article Multidisciplinary Sciences

Molecular understanding of cation effects on double layers and their significance to CO-CO dimerization

Jia-Bo Le et al.

Summary: In this study, the effects of cations on the structure and capacitance of electric double layers were systematically investigated through ab initio molecular dynamics simulations. The computed results were in quantitative agreement with experiments, indicating a clear correlation between the size and hydration energy of cations and the capacitance trend. The Helmholtz capacitance was found to be a key descriptor for measuring the activity of CO-CO dimerization.

NATIONAL SCIENCE REVIEW (2023)

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Article Chemistry, Multidisciplinary

Zooming into the Inner Helmholtz Plane of Pt(111)-Aqueous Solution Interfaces: Chemisorbed Water and Partially Charged Ions

Jun Huang

Summary: The double layer on transition metals, such as platinum, exhibits metal-solvent interactions and partially charged chemisorbed ions. A refined model is proposed that considers a continuous spectrum of solvent molecules, partially charged ions, and different planes for chemisorbed ions and solvent molecules. The model offers an alternative interpretation for capacitance data of Pt(111)-aqueous solution interfaces and raises questions about the existence of a pure double-layer region on a realistic Pt(111) surface.

JACS AU (2023)

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Article Chemistry, Multidisciplinary

The Role of Cation Acidity on the Competition between Hydrogen Evolution and CO2 Reduction on Gold Electrodes

Mariana C. O. Monteiro et al.

Summary: The presence of multivalent cations has been shown to affect CO2 electroreduction and competing hydrogen evolution reactions, with acidic cations favoring CO2RR at low overpotentials in acidic media. Cation acidity correlates with the activity and onset of the water reduction reaction, with weakly hydrated trivalent species exhibiting the highest activity. Among the nonacidic cations, Cs+, Ba2+, and Nd3+ show coordination to adsorbed CO2, enabling stabilization of the *CO2- intermediate and barrierless protonation to COOH and other reduction products.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Multidisciplinary Sciences

Double-layer structure of the Pt(111)-aqueous electrolyte interface

Kasinath Ojha et al.

Summary: This study presents detailed measurements of the double-layer capacitance at the Pt(111)-electrolyte interface near the potential of zero charge (PZC). Strong deviations from traditional Gouy-Chapman-Stern behavior are observed at low electrolyte concentrations, independent of the nature of the electrolyte ions. The capacitance further away from PZC and the trends for increasing ion concentration show ion-specific effects related to ion size or hydration strength. A model is formulated to explain the structure of the electric double layer at the Pt(111)-electrolyte interface, going beyond the Gouy-Chapman-Stern theory.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2022)

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Article Multidisciplinary Sciences

On the importance of the electric double layer structure in aqueous electrocatalysis

Seung-Jae Shin et al.

Summary: This study demonstrates the successful reproduction of experimental capacitance peaks through first-principles molecular simulation, revealing the origins of these peaks and the effect of cation complexation on carbon dioxide reduction activity. The research bridges the mechanistic gap between the electric double layer structure and electrocatalysis, highlighting the catalytic importance of the complex structural response of the EDL.

NATURE COMMUNICATIONS (2022)

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Article Chemistry, Physical

OH Binding Energy as a Universal Descriptor of the Potential of ZeroCharge on Transition Metal Surfaces

Sara R. Kelly et al.

Summary: In this study, ab initio molecular dynamics simulations are used to investigate the characteristics of various transition metal-water interfaces and find simple descriptors for predicting the potential of zero charge. A good correlation is found between water coverage and the reduction of work function, and the vacuum binding energies of H2O and *OH species are determined to be good descriptors for predicting water coverage and the reduction of work function. The findings provide insights into different facet geometries and mixed metal surfaces, and a scheme to predict the potential of zero charge based on *OH binding and the vacuum work function is proposed.

JOURNAL OF PHYSICAL CHEMISTRY C (2022)

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Article Chemistry, Physical

Modulating electric field distribution by alkali cations for CO2 electroreduction in strongly acidic medium

Jun Gu et al.

Summary: This study demonstrates that efficient CO2 electroreduction can be achieved in acidic medium by suppressing hydrogen evolution using alkali cations, overcoming the limitations caused by carbonate formation. The effects of cations are applicable to various catalysts and are achieved by modifying the electric field distribution and stabilizing key intermediates.

NATURE CATALYSIS (2022)

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Article Chemistry, Physical

Correlating hydration free energy and specific adsorption of alkali metal cations during CO2 electroreduction on Au

Vincent J. Ovalle et al.

Summary: This study used the vibration band of tetramethylammonium as a probe to monitor the displacement of specifically adsorbed tetramethylammonium by alkali metal cations. The observed surface coverages of alkali metal cations correlated with their free energies of hydration and the rate of CO2-to-CO conversion.

NATURE CATALYSIS (2022)

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Article Chemistry, Physical

Helmholtz Capacitance of Aqueous NaCl Solutions at the Au(100) Electrode from Polarizable and Nonpolarizable Molecular Dynamics Simulations

Jesse G. McDaniel et al.

Summary: Aqueous NaCl solutions at gold electrodes serve as prototypical electrochemical interfaces. Computer simulations can help interpret electrochemical capacitance data, and our study found that the inner layer capacitance can be described by a generalized Helmholtz model.

JOURNAL OF PHYSICAL CHEMISTRY C (2022)

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Article Chemistry, Physical

Hydrogen bond network connectivity in the electric double layer dominates the kinetic pH effect in hydrogen electrocatalysis on Pt

Peng Li et al.

Summary: This study investigates the origin of the large kinetic pH effect in hydrogen electrocatalysis and reveals the significant difference in the connectivity of hydrogen-bond networks in electric double layers between acid and alkaline environments. The research shows that OH adsorption plays a crucial role in improving the kinetics of alkaline hydrogen electrocatalysis by increasing the connectivity of hydrogen-bond networks. These findings emphasize the importance of electric double layer structures in electrocatalysis.

NATURE CATALYSIS (2022)

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Article Chemistry, Physical

The role of alkali metal cations and platinum-surface hydroxyl in the alkaline hydrogen evolution reaction

Aamir Hassan Shah et al.

Summary: The kinetics of platinum-catalysed hydrogen evolution reaction (HER) in alkaline electrolyte is poor, mainly due to the complexity of the platinum-water interface caused by the presence of alkali metal cations. The alkali metal cations have different effects on the destabilization of hydroxyl adsorbate species, which in turn affects the HER kinetics.

NATURE CATALYSIS (2022)

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Article Chemistry, Physical

Hydrogen Coupling on Platinum Using Artificial Neural Network Potentials and DFT

Peter S. Rice et al.

Summary: Understanding reactions at solid-liquid interfaces is challenging, and controlling solvent-substrate interactions is crucial for developing catalysts beyond platinum.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2021)

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Article Chemistry, Physical

Establishment of the Potential of Zero Charge of Metals in Aqueous Solutions: Different Faces of Water Revealed by Ab Initio Molecular Dynamics Simulations

Peng Li et al.

Summary: Metal-water interactions were studied through molecular dynamics simulations on Pt(111) and Au(111) surfaces interfaced with water, revealing that first layer water molecules decrease the metal work function while second layer water molecules increase it. Introducing chemisorbed hydrogen with varying coverages modulates the metal-water interactions.

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

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Article Physics, Multidisciplinary

Dielectric Properties of Nanoconfined Water: A Canonical Thermopotentiostat Approach

F. Deissenbeck et al.

Summary: Our novel approach samples the canonical ensemble at constant temperature and applied electric potential, easily implemented in any density-functional theory code. Using thermopotentiostat molecular dynamics simulations, we can calculate the dielectric constant of nanoconfined water without assumptions for dielectric volume. Compared to traditional methods, our technique reduces computational time significantly.

PHYSICAL REVIEW LETTERS (2021)

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Article Chemistry, Physical

Modeling the Gouy-Chapman Diffuse Capacitance with Attractive Ion-Surface Interaction

Katharina Doblhoff-Dier et al.

Summary: "Recent experiments have shown deviations from the Gouy-Chapman behavior even in dilute electrolytes on platinum and gold single-crystal electrodes, attributed to an interaction between the surface and the electrolyte ions. A proposed double-layer model reproduces experimental findings and infers characteristics of the ion-surface interaction, suggesting the attractive interaction to be weaker than typical chemical bonds formed during contact adsorption and similar for all ions."

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

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Article Chemistry, Physical

Linear Correlation between Water Adsorption Energies and Volta Potential Differences for Metal/water Interfaces

Xiang-Ying Li et al.

Summary: The study reveals a linear correlation between the adsorption energy of water on metal surface and the interface potential difference, with the adsorption energy determining the coverage of chemisorbed water and influencing the interface potential change.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2021)

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Article Chemistry, Physical

Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution

Mariana C. O. Monteiro et al.

Summary: The study found that metal cations play a crucial role in stabilizing the CO2 intermediate during the reduction process on gold electrodes. Density functional theory simulations confirmed that partially desolvated metal cations enable the reduction by stabilizing the CO2- intermediate through short-range electrostatic interactions. In conclusion, the positively charged species from the electrolyte are key to stabilizing the crucial reaction intermediate.

NATURE CATALYSIS (2021)

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Article Chemistry, Multidisciplinary

Modeling Electrified Pt(111)-Had/Water Interfaces from Ab Initio Molecular Dynamics

Jia-Bo Le et al.

Summary: This study utilized advanced computational methods to simulate and analyze the electric double layers (EDL) of the electrified Pt(1 1 1)-H-ad/water interface, obtaining results that agree with experiments and providing a solid basis for understanding electrochemical processes.

JACS AU (2021)

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Article Chemistry, Multidisciplinary

Double Layer of Pt(111)-Aqueous Electrolyte Interface: Potential of Zero Charge and Anomalous Gouy-Chapman Screening

Kasinath Ojha et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Multidisciplinary Sciences

Molecular origin of negative component of Helmholtz capacitance at electrified Pt(111)/water interface

Jia-Bo Le et al.

SCIENCE ADVANCES (2020)

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Article Chemistry, Physical

In situ probing electrified interfacial water structures at atomically flat surfaces

Chao-Yu Li et al.

NATURE MATERIALS (2019)

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Article Chemistry, Physical

Computational Ag/AgCl Reference Electrode from Density Functional Theory-Based Molecular Dynamics

Xiao-Hui Yang et al.

JOURNAL OF PHYSICAL CHEMISTRY B (2019)

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Article Electrochemistry

How cations determine the interfacial potential profile: Relevance for the CO2 reduction reaction

Ghulam Hussain et al.

ELECTROCHIMICA ACTA (2019)

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Article Chemistry, Physical

Structure and Dynamics of the Liquid-Water/Zinc-Oxide Interface from Machine Learning Potential Simulations

Vanessa Quaranta et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2019)

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Article Chemistry, Physical

Atomic-Scale Simulation of Electrochemical Processes at Electrode/Water Interfaces under Referenced Bias Potential

Assil Bouzid et al.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2018)

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Article Chemistry, Physical

Electrochemical Capacitance of CO-Terminated Pt(111) Dominated by the CO-Solvent Gap

Ravishankar Sundararaman et al.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2017)

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Article Chemistry, Physical

Electrode potential dependent desolvation and resolvation of germanium(100) in contact with aqueous perchlorate electrolytes

Fang Niu et al.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2017)

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Article Physics, Multidisciplinary

Determining Potentials of Zero Charge of Metal Electrodes versus the Standard Hydrogen Electrode from Density-Functional-Theory-Based Molecular Dynamics

Jiabo Le et al.

PHYSICAL REVIEW LETTERS (2017)

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Article Multidisciplinary Sciences

Properties of real metallic surfaces: Effects of density functional semilocality and van der Waals nonlocality

Abhirup Patra et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2017)

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Article Energy & Fuels

Interfacial water reorganization as a pH-dependent descriptor of the hydrogen evolution rate on platinum electrodes

Isis Ledezma-Yanez et al.

NATURE ENERGY (2017)

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Review Chemistry, Multidisciplinary

Redox Potentials and Acidity Constants from Density Functional Theory Based Molecular Dynamics

Jun Cheng et al.

ACCOUNTS OF CHEMICAL RESEARCH (2014)

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Article Chemistry, Physical

Ab initio molecular dynamics study of the Helmholtz layer formed on solid-liquid interfaces and its capacitance

Yasunobu Ando et al.

CHEMICAL PHYSICS LETTERS (2013)

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Article Chemistry, Physical

Alignment of electronic energy levels at electrochemical interfaces

Jun Cheng et al.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2012)

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Article Materials Science, Multidisciplinary

Standard hydrogen electrode and potential of zero charge in density functional calculations

Vladimir Tripkovic et al.

PHYSICAL REVIEW B (2011)

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Article Physics, Multidisciplinary

Generalized neural-network representation of high-dimensional potential-energy surfaces

Joerg Behler et al.

PHYSICAL REVIEW LETTERS (2007)

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Article Chemistry, Physical

Measurement of the surface charge density of CO-saturated Pt(111) electrodes as a function of potential: the potential of zero charge of Pt(111)

A Cuesta

SURFACE SCIENCE (2004)

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Article Electrochemistry

Double layer capacitance of Pt(111) single crystal electrodes

T Pajkossy et al.

ELECTROCHIMICA ACTA (2001)

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