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Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example

[Image: see text] Molecular dynamics simulations are a powerful tool to study diffusion processes in battery electrolyte and electrode materials. From molecular dynamics simulations, many properties relevant to diffusion can be obtained, including the diffusion path, amplitude of vibrations, jump ra...

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Autores principales: de Klerk, Niek J.J., van der Maas, Eveline, Wagemaker, Marnix
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2018
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6058286/
https://www.ncbi.nlm.nih.gov/pubmed/30057999
http://dx.doi.org/10.1021/acsaem.8b00457
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author de Klerk, Niek J.J.
van der Maas, Eveline
Wagemaker, Marnix
author_facet de Klerk, Niek J.J.
van der Maas, Eveline
Wagemaker, Marnix
author_sort de Klerk, Niek J.J.
collection PubMed
description [Image: see text] Molecular dynamics simulations are a powerful tool to study diffusion processes in battery electrolyte and electrode materials. From molecular dynamics simulations, many properties relevant to diffusion can be obtained, including the diffusion path, amplitude of vibrations, jump rates, radial distribution functions, and collective diffusion processes. Here it is shown how the activation energies of different jumps and the attempt frequency can be obtained from a single molecular dynamics simulation. These detailed diffusion properties provide a thorough understanding of diffusion in solid electrolytes, and provide direction for the design of improved solid electrolyte materials. The presently developed analysis methodology is applied to DFT MD simulations of Li-ion diffusion in β-Li(3)PS(4). The methodology presented is generally applicable to diffusion in crystalline materials and facilitates the analysis of molecular dynamics simulations. The code used for the analysis is freely available at: https://bitbucket.org/niekdeklerk/md-analysis-with-matlab. The results on β–Li(3)PS(4) demonstrate that jumps between bc planes limit the conductivity of this important class of solid electrolyte materials. The simulations indicate that the rate-limiting jump process can be accelerated significantly by adding Li interstitials or Li vacancies, promoting three-dimensional diffusion, which results in increased macroscopic Li-ion diffusivity. Li vacancies can be introduced through Br doping, which is predicted to result in an order of magnitude larger Li-ion conductivity in β–Li(3)PS(4). Furthermore, the present simulations rationalize the improved Li-ion diffusivity upon O doping through the change in Li distribution in the crystal. Thus, it is demonstrated how a thorough understanding of diffusion, based on thorough analysis of MD simulations, helps to gain insight and develop strategies to improve the ionic conductivity of solid electrolytes.
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spelling pubmed-60582862018-07-26 Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example de Klerk, Niek J.J. van der Maas, Eveline Wagemaker, Marnix ACS Appl Energy Mater [Image: see text] Molecular dynamics simulations are a powerful tool to study diffusion processes in battery electrolyte and electrode materials. From molecular dynamics simulations, many properties relevant to diffusion can be obtained, including the diffusion path, amplitude of vibrations, jump rates, radial distribution functions, and collective diffusion processes. Here it is shown how the activation energies of different jumps and the attempt frequency can be obtained from a single molecular dynamics simulation. These detailed diffusion properties provide a thorough understanding of diffusion in solid electrolytes, and provide direction for the design of improved solid electrolyte materials. The presently developed analysis methodology is applied to DFT MD simulations of Li-ion diffusion in β-Li(3)PS(4). The methodology presented is generally applicable to diffusion in crystalline materials and facilitates the analysis of molecular dynamics simulations. The code used for the analysis is freely available at: https://bitbucket.org/niekdeklerk/md-analysis-with-matlab. The results on β–Li(3)PS(4) demonstrate that jumps between bc planes limit the conductivity of this important class of solid electrolyte materials. The simulations indicate that the rate-limiting jump process can be accelerated significantly by adding Li interstitials or Li vacancies, promoting three-dimensional diffusion, which results in increased macroscopic Li-ion diffusivity. Li vacancies can be introduced through Br doping, which is predicted to result in an order of magnitude larger Li-ion conductivity in β–Li(3)PS(4). Furthermore, the present simulations rationalize the improved Li-ion diffusivity upon O doping through the change in Li distribution in the crystal. Thus, it is demonstrated how a thorough understanding of diffusion, based on thorough analysis of MD simulations, helps to gain insight and develop strategies to improve the ionic conductivity of solid electrolytes. American Chemical Society 2018-06-12 2018-07-23 /pmc/articles/PMC6058286/ /pubmed/30057999 http://dx.doi.org/10.1021/acsaem.8b00457 Text en Copyright © 2018 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle de Klerk, Niek J.J.
van der Maas, Eveline
Wagemaker, Marnix
Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example
title Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example
title_full Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example
title_fullStr Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example
title_full_unstemmed Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example
title_short Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-Li(3)PS(4) as an Example
title_sort analysis of diffusion in solid-state electrolytes through md simulations, improvement of the li-ion conductivity in β-li(3)ps(4) as an example
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6058286/
https://www.ncbi.nlm.nih.gov/pubmed/30057999
http://dx.doi.org/10.1021/acsaem.8b00457
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