Understanding the Electric Double-Layer Structure, Capacitance, and Charging Dynamics

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(12), P. 10821 - 10859

Published: May 20, 2022

Significant progress has been made in recent years theoretical modeling of the electric double layer (EDL), a key concept electrochemistry important for energy storage, electrocatalysis, and multitudes other technological applications. However, major challenges remain understanding microscopic details electrochemical interface charging mechanisms under realistic conditions. This review delves into methods to describe equilibrium dynamic responses EDL structure capacitance systems commonly deployed capacitive storage. Special emphasis is given advances that intend capture nonclassical behavior such as oscillatory ion distributions, polarization nonmetallic electrodes, charge transfer, various forms phase transitions micropores electrodes interfacing with an organic electrolyte or ionic liquid. comprehensive analysis highlights insights predictable relationships between materials characteristics performance offers perspective on opportunities further development toward rational design optimization systems.

Language: Английский

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Developing high safety Li-metal anodes for future high-energy Li-metal batteries: strategies and perspectives

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(15), P. 5407 - 5445

Published: Jan. 1, 2020

Developing high-safety Li-metal anodes (LMAs) are extremely important for the application of high-energy batteries. The recently state-of-the-art technologies, strategies and perspectives developing LMAs comprehensively summarized in this review.

Language: Английский

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Machine Learning for Electronically Excited States of Molecules

Chemical Reviews, Journal Year: 2020, Volume and Issue: 121(16), P. 9873 - 9926

Published: Nov. 19, 2020

Electronically excited states of molecules are at the heart photochemistry, photophysics, as well photobiology and also play a role in material science. Their theoretical description requires highly accurate quantum chemical calculations, which computationally expensive. In this review, we focus on not only how machine learning is employed to speed up such excited-state simulations but branch artificial intelligence can be used advance exciting research field all its aspects. Discussed applications for include dynamics simulations, static calculations absorption spectra, many others. order put these studies into context, discuss promises pitfalls involved techniques. Since latter mostly based chemistry provide short introduction electronic structure methods approaches nonadiabatic describe tricks problems when using them molecules.

Language: Английский

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Artificial Intelligence Applied to Battery Research: Hype or Reality?

Chemical Reviews, Journal Year: 2021, Volume and Issue: 122(12), P. 10899 - 10969

Published: Sept. 16, 2021

This is a critical review of artificial intelligence/machine learning (AI/ML) methods applied to battery research. It aims at providing comprehensive, authoritative, and critical, yet easily understandable, general interest the community. addresses concepts, approaches, tools, outcomes, challenges using AI/ML as an accelerator for design optimization next generation batteries─a current hot topic. intends create both accessibility these tools chemistry electrochemical energy sciences communities completeness in terms different R&D aspects covered.

Language: Английский

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Applying Classical, Ab Initio, and Machine-Learning Molecular Dynamics Simulations to the Liquid Electrolyte for Rechargeable Batteries

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(12), P. 10970 - 11021

Published: May 16, 2022

Rechargeable batteries have become indispensable implements in our daily life and are considered a promising technology to construct sustainable energy systems the future. The liquid electrolyte is one of most important parts battery extremely critical stabilizing electrode–electrolyte interfaces constructing safe long-life-span batteries. Tremendous efforts been devoted developing new solvents, salts, additives, recipes, where molecular dynamics (MD) simulations play an increasingly role exploring structures, physicochemical properties such as ionic conductivity, interfacial reaction mechanisms. This review affords overview applying MD study electrolytes for rechargeable First, fundamentals recent theoretical progress three-class summarized, including classical, ab initio, machine-learning (section 2). Next, application exploration electrolytes, probing bulk structures 3), deriving macroscopic conductivity dielectric constant 4), revealing mechanisms 5), sequentially presented. Finally, general conclusion insightful perspective on current challenges future directions provided. Machine-learning technologies highlighted figure out these challenging issues facing research promote rational design advanced next-generation

Language: Английский

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Polarizable embedding QM/MM: the future gold standard for complex (bio)systems?

Physical Chemistry Chemical Physics, Journal Year: 2020, Volume and Issue: 22(26), P. 14433 - 14448

Published: Jan. 1, 2020

We provide a perspective of the induced dipole formulation polarizable QM/MM, showing how efficient implementations will enable their application to modeling dynamics, spectroscopy, and reactivity in complex biosystems.

Language: Английский

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Surface-active ionic liquids: A review

Journal of Molecular Liquids, Journal Year: 2021, Volume and Issue: 347, P. 118160 - 118160

Published: Dec. 1, 2021

The combination of water and surface-active ionic liquids provides a unique reaction medium, facilitating aggregation micellization the liquid to allow for chemical reactions in bulk water. With growing focus on sustainable technologies, have emerged as tunable solvents multiple applications but are often too viscous or expensive use solvent. As result, there has been tremendous increase interest behavior presence It already shown that certain act surfactants aqueous solutions, enabling both afford solvent systems with properties. Ultimately, give rise distinct chemistry their own compared traditional molecular solvents, thus is rapidly growing. In this review, general structure key features micellar structures discussed. Furthermore, characterization techniques formed micelles presented, discussing possible methods studying behavior. Finally, current across all fields chemistry, from organic nanoparticle synthesis presented.

Language: Английский

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“Solvent-in-salt” systems for design of new materials in chemistry, biology and energy research

Chemical Society Reviews, Journal Year: 2018, Volume and Issue: 47(4), P. 1250 - 1284

Published: Jan. 1, 2018

“Solvent-in-salt” (SIS) systems with a very high salt content have recently emerged as potent tools for solution of highly relevant chemical problems.

Language: Английский

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Microscopic Simulations of Electrochemical Double-Layer Capacitors

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(12), P. 10860 - 10898

Published: April 7, 2022

Electrochemical double-layer capacitors (EDLCs) are devices allowing the storage or production of electricity. They function through adsorption ions from an electrolyte on high-surface-area electrodes and characterized by short charging/discharging times long cycle-life compared to batteries. Microscopic simulations now widely used characterize structural, dynamical, properties these devices, complementing electrochemical experiments in situ spectroscopic analyses. In this review, we discuss main families simulation methods that have been developed their application family EDLCs, which include nanoporous carbon electrodes. We focus organic for electricity applications as well aqueous systems context blue energy harvesting desalination. finally provide perspectives further improvement predictive power simulations, particular future with complex electrode compositions.

Language: Английский

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Transferable, Polarizable Force Field for Ionic Liquids

Journal of Chemical Theory and Computation, Journal Year: 2019, Volume and Issue: 15(11), P. 5858 - 5871

Published: Sept. 17, 2019

A general, transferable, polarizable force field for molecular simulation of ionic liquids (ILs) and their mixtures with compounds is developed. This model derived from the widely used CL&P fixed-charge that describes most families ILs, in a form compatible OPLS-AA, one major fields organic compounds. Models ILs fixed, integer-ionic charges lead to pathologically slow dynamics, problem corrected when polarization effects are included explicitly. In proposed here, Drude-induced dipoles parameters determined atomic polarizabilities. The modified upon inclusion Drude avoid double-counting effects. modification based on first-principles calculations dispersion induction contributions van der Waals interactions using symmetry-adapted perturbation theory (SAPT) set dimers composed positive, negative, neutral fragments representative wide variety ILs. fragment approach provides transferability, allowing representation multitude cation anion families, including different functional groups, without need reparametrize. Because SAPT expensive, an alternative predictive scheme was devised, requiring only properties clear physical meaning, namely, dipole moments new field, CL&Pol, broad validated by comparisons experimental data density, ion diffusion coefficients, viscosity. approaches here can also be applied conversion other into versions.

Language: Английский

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