A Holistic Take on Simulating Battery Electrolytes
Doctoral thesis, 2023
The way energy storage materials have been developed up until now have mainly been in the lab. With many other industries benefiting from IT tools the battery industry is seeing a need for new better computational tools to aid in developing new materials. Many put their faith in machine learning algorithms to provide the solution, but those methods are not flawless, and are especially hard to work with when modeling electrolytes. This thesis focuses on physics-based methods to model battery electrolytes, such as DFT, AIMD, and classical MD, and makes a holistic retake on how these methods could be used in unison to better help material developers screen their materials.
Novel electrolyte concepts such as highly concentrated electrolytes and localized highly concentrated electrolytes, both for lithium and calcium batteries, are studied using the aforementioned tools. This thesis also presents how the newly developed CHAMPION software and methods can be used to tie the dierent methods together and possibly also extend their use by mapping forces on identified interatomic interactions, which may enable much faster turn-around in the simulation protocols.
machine learning
lithium-ion batteries
multi-scale modeling
AIMD
MD
electrolytes
DFT
Author
Fabian Årén
Chalmers, Physics, Materials Physics
(Localized) Highly Concentrated Electrolytes for Calcium Batteries
Batteries and Supercaps,;Vol. In Press(2023)
Journal article
CHAMPION: Chalmers hierarchical atomic, molecular, polymeric and ionic analysis toolkit
Journal of Computational Chemistry,;Vol. 42(2021)p. 1632-1642
Journal article
Ion Transport Mechanisms via Time-Dependent Local Structure and Dynamics in Highly Concentrated Electrolytes
Journal of the Electrochemical Society,;Vol. 167(2020)
Journal article
F Årén, R. Andersson, A. Franco, and P. Johansson, “Structure, Dynamics and Ion Transport Mechanisms in Lithium-Ion Battery Electrolytes: Origin and Onset of Highly Concentrated Electrolyte Behavior,”
F. Årén, R. Andersson, and P. Johansson, “Sidestepping the use of molecular dynamics force fields,”
Hittills har denna materialutveckling främst skett genom ett experimentellt dominerat "trial-and-error" tillvägagångssätt. För att effektivisera det arbetet så föreslår denna avhandling hur man mera effektivt kan använda beräkningsmetoder för att bättre guida utvecklingen av elektrolyter. Detta är extra viktigt då mångaproblem har sitt ursprung i just elektrolyten samt att för nya koncept kan beräkningar ge unik information svår att erhålla med experiment.
Highly concentrated electrolytes
Swedish Energy Agency (39909-1), 2015-02-01 -- 2019-09-30.
High energy lithium sulphur cells and batteries (HELIS)
European Commission (EC) (EC/H2020/666221), 2015-06-01 -- 2019-05-31.
CAlcium Rechargeable BAttery Technology (CARBAT)
European Commission (EC) (EC/H2020/766617), 2017-10-01 -- 2020-09-30.
Driving Forces
Sustainable development
Innovation and entrepreneurship
Areas of Advance
Transport
Energy
Materials Science
Subject Categories
Physical Sciences
Materials Chemistry
Vehicle Engineering
Infrastructure
C3SE (Chalmers Centre for Computational Science and Engineering)
ISBN
978-91-7905-862-3
Doktorsavhandlingar vid Chalmers tekniska högskola. Ny serie: 5328
Publisher
Chalmers
PJ
Opponent: Prof. Rafael Gómez-Bombarelli, Massachusetts Institute of Technology, USA