title: First-Principles Density Functional Theory Modeling of Li Binding: Thermodynamics and Redox Properties of Quinone Derivatives for Lithium-Ion Batteries.
abstract: The Li-binding thermodynamics and redox potentials of seven different quinone derivatives are investigated to determine their suitability as positive electrode materials for lithium-ion batteries. First, using density functional theory (DFT) calculations on the interactions between the quinone derivatives and Li atoms, we find that the Li atoms primarily bind with the carbonyl groups in the test molecules. Next, we observed that the redox properties of the quinone derivatives can be tuned in the desired direction by systematically modifying their chemical structures using electron-withdrawing functional groups. Further, DFT-based investigations of the redox potentials of the Li-bound quinone derivatives provide insights regarding the changes induced in their redox properties during the discharging process. The redox potential decreases as the number of bound Li atoms is increased. However, we found that the functionalization of the quinone derivatives with carboxylic acids can improve their redox potential as well as their charge capacity. Through this study, we also determined that the cathodic activity of quinone derivatives during the discharging process relies strongly on the solvation effect as well as on the number of carbonyl groups available for further Li binding.
authors.affiliation: Computational NanoBio Technology Laboratory, School of Materials Science and Engineering, Georgia Institute of Technology , 771 Ferst Drive NW, Atlanta, Georgia 30332-0245, United States.
authors.forename: Ki Chul
authors.initials: KC
authors.lastname: Kim
authors.affiliation: G. W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology , Atlanta, Georgia 30332-0405, United States.
authors.forename: Tianyuan
authors.initials: T
authors.lastname: Liu
authors.affiliation: G. W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology , Atlanta, Georgia 30332-0405, United States.|Institute for Electronics and Nanotechnology, Georgia Institute of Technology , Atlanta, Georgia 30332, United States.
authors.forename: Seung Woo
authors.initials: SW
authors.lastname: Lee
authors.affiliation: Computational NanoBio Technology Laboratory, School of Materials Science and Engineering, Georgia Institute of Technology , 771 Ferst Drive NW, Atlanta, Georgia 30332-0245, United States.|Institute for Electronics and Nanotechnology, Georgia Institute of Technology , Atlanta, Georgia 30332, United States.|Parker H. Petit Institute for Bioengineering and Bioscience, Georgia Institute of Technology , Atlanta, Georgia 30332-0363, United States.
authors.forename: Seung Soon
authors.initials: SS
authors.lastname: Jang