Characterizing microscale single particles directly is requested for dissecting the performance-limiting factors at the electrode scale. In this work, we build a single-particle electrochemical setup and develop a physics-based model for extracting the solid-phase diffusion coefficient (D ) and exchange current density (i ) from electrochemical impedance measurements. We find that the carbon coating on the LiNi Mn Co O surface enhances i . In addition, D and i decay irreversibly by ≈25 % and ≈10 %, respectively, when the cutoff charge voltage increases from 4.3 V to 4.4 V. Moreover, we correlate intrinsic parameters of single particles with the performance of porous electrodes. Porous electrodes assembled with active particles with higher i values deliver a greater capacity and faster capacity fade. The methods developed in this combined experimental and theoretical work can be useful in correlating the single-particle scale and porous-electrode scale for other similar systems.
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http://dx.doi.org/10.1002/anie.202205394 | DOI Listing |
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