State‐of‐Charge Distribution of Single‐Crystalline NMC532 Cathodes in Lithium‐Ion Batteries: A Critical Look at the Mesoscale

The electrochemical response of layered lithium transition metal oxides LiMO2 [M=Ni, Mn, Co; e. g., Li(Ni0.5Mn0.3Co0.2)O2 (NMC532)] with single‐crystalline architecture to slow and fast charging protocols and the implication of incomplete and heterogeneous redox reactions on the active material util...

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Bibliographic Details
Published in:ChemSusChem 2022-11, Vol.15 (21), p.e202201169-n/a
Main Authors: Kröger, Till‐Niklas, Wölke, Mathis Jan, Harte, Patrick, Beuse, Thomas, Winter, Martin, Nowak, Sascha, Wiemers‐Meyer, Simon
Format: Article
Language:English
Subjects:
Charge distribution
electrochemistry
Electrodes
energy storage
Evolution
Failure mechanisms
Heterogeneity
Inductively coupled plasma
Lithium-ion batteries
Optical emission spectroscopy
particle size
Redox reactions
Single crystals
State of charge
Transition metal oxides
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Summary:The electrochemical response of layered lithium transition metal oxides LiMO2 [M=Ni, Mn, Co; e. g., Li(Ni0.5Mn0.3Co0.2)O2 (NMC532)] with single‐crystalline architecture to slow and fast charging protocols and the implication of incomplete and heterogeneous redox reactions on the active material utilization during cycling were the subject of this work. The role of the active material size and the influence of the local microstructural and chemical ramifications in the composite electrode on the evolution of heterogeneous state of charge (SOC) distribution were deciphered. For this, classification‐single‐particle inductively coupled plasma optical emission spectroscopy (CL‐SP‐ICP‐OES) was comprehensively supplemented by various post mortem analytical techniques. The presented results question the impact of surface‐dependent failure mechanisms of single crystals for the evolution of SOC heterogeneity and identify the deficient structural flexibility of the composite electrode framework as the main driver for the observed non‐uniform active material utilization. State of charge: The particle size‐ and rate‐dependent evolution of persistent mesoscale state‐of‐charge heterogeneity is revealed upon different cycling protocols for NMC532 with single‐crystalline architecture. The structural fatigue of the composite matrix is concluded to be the main driver for the observed non‐uniform active material utilization.
ISSN:1864-5631
1864-564X
1864-564X
DOI:10.1002/cssc.202201169