Quantum-Chemical Study of the FeNCN Conversion-Reaction Mechanism in Lithium- and Sodium-Ion Batteries.
Angew Chem Int Ed Engl
; 59(9): 3718-3723, 2020 Feb 24.
Article
em En
| MEDLINE
| ID: mdl-31828910
ABSTRACT
We report a computational study on 3d transition-metal (Cr, Mn, Fe, and Co) carbodiimides in Li- and Na-ion batteries. The obtained cell voltages semi-quantitatively fit the experiments, highlighting the practicality of PBE+U as an approach for modeling the conversion-reaction mechanism of the FeNCN archetype with lithium and sodium. Also, the calculated voltage profiles agree satisfactorily with experiment both for full (Li-ion battery) and partial (Na-ion battery) discharge, even though experimental atomistic knowledge is missing up to now. Moreover, we rationalize the structural preference of intermediate ternaries and their characteristic lowering in the voltage profile using chemical-bonding and Mulliken-charge analysis. The formation of such ternary intermediates for the lithiation of FeNCN and the contribution of at least one ternary intermediate is also confirmed experimentally. This theoretical approach, aided by experimental findings, supports the atomistic exploration of electrode materials governed by conversion reactions.
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1
Base de dados:
MEDLINE
Tipo de estudo:
Prognostic_studies
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2020
Tipo de documento:
Article
País de afiliação:
Alemanha