Tuning the Electrochemical Properties of Organic Battery Cathode Materials: Insights from Evolutionary Algorithm DFT Calculations.
Rodrigo P CarvalhoCleber Fabiano do Nascimento MarchioriDaniel BrandellCarlos Moyses AraujoPublished in: ChemSusChem (2020)
Several forms of organic materials have arisen as promising candidates for future active electrode materials for Li-ion and post-Li-ion batteries, owing to a series of key features that encompasses sustainability, accessibility, and tunable electrochemical properties by molecular modifications. In this context, a series of organic electrode materials (OEMs) are investigated to further understand their thermodynamic and electronic properties. Through an evolutionary algorithm approach combined with first-principles calculations, the crystal structure of lithiated and delithiated phases of these OEMs and their respective NO2 -substituted analogues are predicted. This framework allows a first assessment of their electrochemical and electronic properties and further understanding on the effects of the nitro group in the substituted compounds. NO2 is found to strongly affect structural and thermodynamic aspects during the electrochemical reaction with the reducing equivalents (Li+ +e- ), changing the OEM's character from a low-potential anode to a high-potential cathode by creating a localization of the additional electrons, thus resulting in a better-defined redox-active center and leading to a shift in the potential from 0.92 V to 2.66 V vs. Li/Li+ .
Keyphrases
- ion batteries
- gold nanoparticles
- molecular docking
- molecularly imprinted
- density functional theory
- ionic liquid
- label free
- machine learning
- molecular dynamics simulations
- electron transfer
- molecular dynamics
- deep learning
- genome wide
- water soluble
- gene expression
- mass spectrometry
- current status
- carbon nanotubes
- monte carlo
- atomic force microscopy
- crystal structure
- tandem mass spectrometry