DFT modelling of explicit solid-solid interfaces in batteries: methods and challenges.

Area of Science:

• Computational materials science
• Electrochemistry
• Energy storage

Background:

• Density Functional Theory (DFT) is standard for bulk electrode properties in lithium batteries.
• DFT modeling of explicit battery interfaces lacks standardized methodology and requires further development.

Purpose of the Study:

• To highlight the critical role of explicit interface models in understanding battery behavior.
• To address key challenges in modeling "dirty" electrode surfaces, voltage control, and kinetic vs. thermodynamic interfacial structures.

Main Methods:

• Utilized Density Functional Theory (DFT) calculations.
• Focused on modeling solid-solid interfaces relevant to all-solid-state and liquid-electrolyte batteries.
• Employed metal anode calculations as illustrative examples.

Main Results:

• Demonstrated that explicit interface models are essential for elucidating contact potentials and electric fields.
• Showcased the importance of interface models for assessing kinetic stability against parasitic reactions.
• Identified "dirty" surfaces, voltage calibration, and kinetics-driven structures as key challenges.

Conclusions:

• Explicit interface modeling is critical for advancing battery technology, particularly for understanding interfacial phenomena.
• New computational techniques and cross-disciplinary insights are needed to overcome current modeling challenges.
• Accurate modeling of battery interfaces will accelerate the development of high energy density storage devices.