Insertion of Mono- vs. Bi- vs. Trivalent Atoms in Prospective Active Electrode Materials for Electrochemical Batteries: An ab Initio Perspective

Vadym V. Kulish, Daniel Koch and Sergei Manzhos
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Vadym V. Kulish: Department of Mechanical Engineering, Faculty of Engineering, National University of Singapore, Block EA #07-08, 9 Engineering Drive 1, Singapore 117576, Singapore
Daniel Koch: Department of Mechanical Engineering, Faculty of Engineering, National University of Singapore, Block EA #07-08, 9 Engineering Drive 1, Singapore 117576, Singapore
Sergei Manzhos: Department of Mechanical Engineering, Faculty of Engineering, National University of Singapore, Block EA #07-08, 9 Engineering Drive 1, Singapore 117576, Singapore

Energies, 2017, vol. 10, issue 12, 1-32

Abstract: Rational design of active electrode materials is important for the development of advanced lithium and post-lithium batteries. Ab initio modeling can provide mechanistic understanding of the performance of prospective materials and guide design. We review our recent comparative ab initio studies of lithium, sodium, potassium, magnesium, and aluminum interactions with different phases of several actively experimentally studied electrode materials, including monoelemental materials carbon, silicon, tin, and germanium, oxides TiO 2 and V x O y as well as sulphur-based spinels MS 2 (M = transition metal). These studies are unique in that they provided reliable comparisons, i.e., at the same level of theory and using the same computational parameters, among different materials and among Li, Na, K, Mg, and Al. Specifically, insertion energetics (related to the electrode voltage) and diffusion barriers (related to rate capability), as well as phononic effects, are compared. These studies facilitate identification of phases most suitable as anode or cathode for different types of batteries. We highlight the possibility of increasing the voltage, or enabling electrochemical activity, by amorphization and p -doping, of rational choice of phases of oxides to maximize the insertion potential of Li, Na, K, Mg, Al, as well as of rational choice of the optimum sulfur-based spinel for Mg and Al insertion, based on ab initio calculations. Some methodological issues are also addressed, including construction of effective localized basis sets, applications of Hubbard correction, generation of amorphous structures, and the use of a posteriori dispersion corrections.

Keywords: lithium ion battery; sodium ion battery; potassium ion battery; magnesium ion battery; aluminum ion battery; intercalation; diffusion; ab initio modeling; energy storage (search for similar items in EconPapers)
JEL-codes: Q Q0 Q4 Q40 Q41 Q42 Q43 Q47 Q48 Q49 (search for similar items in EconPapers)
Date: 2017
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