Abstract
Lithium-ion batteries (LiBs) have gained a worldwide position as energy storage devices due to their high energy density, power density and cycle life. Nevertheless, these performance parameters are yet insufficient for current and future demands diversifying their range of applications, and competitiveness against other power sources. In line with the materials science, the optimization of LiBs, first, requires an in-depth characterization and understanding of their determining steps regarding transport phenomena and electrode kinetics occurring within these devices. Experimental and theoretical studies have identified the solid-state diffusion of Li+ into the composite cathode material as one of the transport mechanisms limiting the performance of LiBs, in particular at high charge and discharge rates (C-rates). Nowadays, there is however ambivalence to characterize this mass transport mechanism using the diffusion coefficient calculated either by electrochemical techniques or ab initio quantum chemistry methods. This contribution revisits conventional electrochemical methodologies employed in literature to estimate mass transport diffusivity of LiBs, in particular using LiFePO4 in the cathode, and their suitability and reliability are comprehensively discussed. These experimental and theoretical methods include Galvanostatic and Potentiostatic Intermittent Titration Technique (GITT and PITT), Electrochemical Impedance Spectroscopy (EIS), Cyclic Voltammetry (CV) and ab initio quantum chemistry methods. On the one hand, experimental methods seem not to isolate the diffusion mechanism in the solid phase; thus, obtaining an unreliable apparent diffusion coefficient (ranging from 10–10 to 10–16 cm2 s−1), which only serves as a criterion to discard among a set of LiBs. On the other hand, atomistic approaches based on ab initio, density functional theory (DFT), cannot yet capture the complexity of the local environments involved at this scale; in consequence, these approaches have predicted inadequate diffusion coefficients for LiFePO4 (ranging from 10–6 to 10–7 cm2 s−1) which strongly differ from experimental values. This contribution, at long last, remarks the factors influencing diffusion mechanisms and addresses the uncertainties to characterize this transport mechanism in the cathode, stressing the needs to establish methods to determine the diffusion coefficient accurately, coupling electrochemical techniques, ab initio methods, and engineering approaches based on modeling.
Abbreviations
- LiBs
Lithium-ion batteries
- GITT
Galvanostatic Intermittent Titration Technique
- PITT
Potentiostatic Intermittent Titration Technique
- EIS
Electrochemical Impedance Spectroscopy
- CV
Cyclic Voltammetry
- DFT
Density Functional Theory
- PVDF
polyvinylidene fluoride
- HFP
hexafluoropropylene
- EC
Ethylene Carbonate
- DEC
Diethyl Carbonate
- DMC
Dimethyl Carbonate
- MSD
Means Square Displacement
- HOMO
Highest occupied molecular orbital
- LUMO
Lowest unoccupied molecular orbital.
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