Robust training of machine learning interatomic potentials with dimensionality reduction and stratified sampling

npj Computational Materials, Journal Year: 2024, Volume and Issue: 10(1)

Published: Feb. 26, 2024

Abstract Machine learning interatomic potentials (MLIPs) enable accurate simulations of materials at scales beyond that accessible by ab initio methods and play an increasingly important role in the study design materials. However, MLIPs are only as robust data on which they trained. Here, we present DImensionality-Reduced Encoded Clusters with sTratified (DIRECT) sampling approach to select a training set structures from large complex configuration space. By applying DIRECT Materials Project relaxation trajectories dataset over one million 89 elements, develop improved 3-body graph network (M3GNet) universal potential extrapolates more reliably unseen structures. We further show molecular dynamics (MD) M3GNet can be used instead expensive MD rapidly create space for target systems. combined this scheme reliable moment tensor titanium hydrides without need iterative augmentation This work paves way high-throughput development across any compositional complexity.

Language: Английский

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Computational approach inspired advancements of solid-state electrolytes for lithium secondary batteries: from first-principles to machine learning

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(6), P. 3134 - 3166

Published: Jan. 1, 2024

The utilization of computational approaches at various scales, including first-principles calculations, MD simulations, multi-physics modeling, and machine learning techniques, has been instrumental in expediting the advancement SSEs.

Language: Английский

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Reversible Enhancement of Electronic Conduction Caused by Phase Transformation and Interfacial Segregation in an Entropy‐Stabilized Oxide

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(25)

Published: Feb. 4, 2024

Abstract Entropy‐stabilized oxide (ESO) research has primarily focused on discovering unprecedented structures, chemistries, and properties in the single‐phase state. However, few studies discuss impacts of entropy stabilization secondary phases functionality particular, electrical conductivity. To address this gap, transport mechanisms canonical ESO rocksalt (Co,Cu,Mg,Ni,Zn)O are assessed as a function phase content. When single‐phase, conducts electrons via Cu + /Cu 2+ small polarons. After 2 h heat treatment, Cu‐rich tenorite form at some grain boundaries (GBs), enhancing interior electronic conductivity by tuning defect chemistry toward higher carrier concentrations. 24 treatment yields all GBs, followed formation anisotropic equiaxed Co‐rich spinel grains, further but slowing across tenorite‐rich GBs. Across samples, total increases (and decreases reversibly) four orders magnitude with heat‐treatment‐induced transformation grains’ concentration lower migration activation energy. This work demonstrates potential to selectively grow grains thereby using microstructure design, nanoscale engineering, paving way develop many novel materials.

Language: Английский

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Porous High-Entropy Oxide Anode Materials for Li-Ion Batteries: Preparation, Characterization, and Applications

Materials, Journal Year: 2024, Volume and Issue: 17(7), P. 1542 - 1542

Published: March 28, 2024

High-entropy oxides (HEOs), as a new type of single-phase solid solution with multi-component design, have shown great potential when they are used anodes in lithium-ion batteries due to four kinds effects (thermodynamic high-entropy effect, the structural lattice distortion kinetic slow diffusion and electrochemical “cocktail effect”), leading excellent cycling stability. Although number articles on study HEO materials has increased significantly, latest research progress porous battery field not been systematically summarized. This review outlines made recent years synthesis, characterization HEOs focuses phase transitions during process, role individual elements, lithium storage mechanisms disclosed through some advanced techniques. Finally, future outlook energy is presented, providing guidance for researchers further improve design HEOs.

Language: Английский

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High-entropy battery materials: Revolutionizing energy storage with structural complexity and entropy-driven stabilization

Materials Science and Engineering R Reports, Journal Year: 2024, Volume and Issue: 163, P. 100921 - 100921

Published: Dec. 17, 2024

Language: Английский

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Tuning grain boundary cation segregation with oxygen deficiency and atomic structure in a perovskite compositionally complex oxide thin film

Applied Physics Letters, Journal Year: 2024, Volume and Issue: 124(17)

Published: April 22, 2024

Compositionally complex oxides (CCOs) are an emerging class of materials encompassing high entropy and stabilized oxides. These promising advanced leverage tunable chemical bond structure, lattice distortion, disorder for unprecedented properties. Grain boundary (GB) point defect segregation to GBs relatively understudied in CCOs even though they can govern macroscopic material For example, GB local (dis)order distribution, playing a critical role electrochemical reaction kinetics, charge mass transport solid electrolytes. However, compared with conventional oxides, multi-cation CCO systems expected exhibit more phenomena and, thus, prove difficult tune through design strategies. Here, was studied model perovskite LaFe0.7Ni0.1Co0.1Cu0.05Pd0.05O3−x textured thin film by (sub-)atomic-resolution scanning transmission electron microscopy imaging spectroscopy. It is found that correlated cation reducibility—predicted Ellingham diagram—as Pd Cu segregate rich oxygen vacancies (VO··). Furthermore, highly sensitive the concentration spatial distribution VO·· along plane, as well fluctuations atomic structure elastic strain induced disorder, such dislocations. This work offers perspective controlling cations tuning reducibility deficiency, which guide CCOs.

Language: Английский

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Lithium dynamics at grain boundaries of β-Li₃PS₄ solid electrolyte

Energy Advances, Journal Year: 2023, Volume and Issue: 2(12), P. 2029 - 2041

Published: Jan. 1, 2023

The lithium diffusivity behavior at the grain boundaries of β-Li 3 PS 4 solid electrolytes is strongly dependent on boundary type and degree disorder.

Language: Английский

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Solid-state electrolytes: a way to increase the power of lithium-ion batteries

Russian Chemical Reviews, Journal Year: 2024, Volume and Issue: 93(6), P. RCR5126 - RCR5126

Published: June 1, 2024

Currently, all-solid-state lithium metal batteries are considered among the most promising energy storage devices, due to their safety and high density. Solid-state electrolytes, key components of batteries, attracting increasing attention. This review presents an analysis important recent advances in field conducting solid-state including mechanisms conductivity, main approaches increase optimization interfaces ways improve stability for types <i>i.e.</i>, inorganic, polymer composite materials. For solid inorganic conductivity have been achieved; however, problems related formation dense thin films a reliable contact with electrode materials still unsolved. Polymer electrolytes characterized by lower which is improved upon plasticization aprotic solvents. Composite it possible achieve combination good mechanical properties along stability, as promising. The solve them outlined.<Br>The bibliography includes 661 references.<Br> Key words: battery, electrolyte, ionic transference numbers

Language: Английский

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Outlook of Solid-State Electrolytes: A Boost in Next-Generation Li-Metal-Based Solid-State Batteries

Energy & Fuels, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 11, 2024

Language: Английский

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A theoretical perspective on solid-state ionic interfaces

Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences, Journal Year: 2024, Volume and Issue: 382(2281)

Published: Sept. 9, 2024

Solid-state ionic conductors find application across various domains in materials science, particularly showcasing their significance energy storage and conversion technologies. To effectively utilize these high-performance electrochemical devices, a comprehensive understanding precise control of charge carriers’ distribution mobility at interfaces are paramount. A major challenge lies unravelling the atomic-level processes governing ion dynamics within intricate solid interfacial structures, such as grain boundaries heterophases. From theoretical viewpoint, this Perspective article, my focus is to offer an overview current comprehension key aspects related solid-state interfaces, with particular emphasis on electrolytes for batteries, while providing personal critical assessment recent research advancements. I begin by introducing fundamental concepts conductors, classical diffusion model chemical potential. Subsequently, delve into modelling space-charge regions, which pivotal physicochemical origins redistribution electrified interfaces. Finally, discuss modern computational methods, density functional theory machine-learned potentials, invaluable tools gaining insights atomic-scale behaviour including both reactivity aspects. This article part theme issue ‘Celebrating 15th anniversary Royal Society Newton International Fellowship’.

Language: Английский

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