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Origin of Aging of a P2-Na$_x$Mn$_{3/4}$Ni$_{1/4}$O$_2$ Cathode Active Material for Sodium-Ion Batteries

Pfeiffer, Lukas Fridolin; Li, Yueliang; Mundszinger, Manuel; Geisler, Jonas; Pfeifer, Claudia; Mikhailova, Daria; Omar, Ahmad; Baran, Volodymyr; Biskupek, Johannes; Kaiser, Ute; Adelhelm, Philipp; Wohlfahrt-Mehrens, Margret; Passerini, Stefano 1; Axmann, Peter
1 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

Sodium-ion batteries (SIB) are currently being developed and commercialized as a promising new technology for cost-effective and powerful electrical energy storage. In this study, we investigate the origin of capacity fading in P2-type layered sodium cathode materials for SIBs using a micron-sized single-crystalline P2-Na$_x$Mn$_{3/4}$Ni$_{1/4}$O$_2$ model cathode active material. Using various electrochemical techniques, we identify the following aging effects upon cycling: (i) a state of charge (SOC)-independent increase in polarization, (ii) a SOC-dependent increase in polarization at high voltage, and (iii) a loss of active material due to electronic disconnection after prolonged cycling. With high-resolution transmission electron microscopy (HRTEM) and energy-dispersive X-ray (EDX) spectroscopy, we identify surface densification, resulting in 5–10 nm thick surface layers on cycled cathode active materials as the origin for SOC-independent increase of polarization. The corresponding oxygen loss is in accordance with gas evolution in differential electrochemical mass spectrometry (DEMS) measurements. Furthermore, with scanning electron microscopy (SEM) electrode cross sections, we identify (partly) reversible cracking at a high SOC as the cause for increased polarization depending on SOC. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000163139
Veröffentlicht am 17.10.2023
Originalveröffentlichung
DOI: 10.1021/acs.chemmater.3c01499
Scopus
Zitationen: 8
Web of Science
Zitationen: 7
Dimensions
Zitationen: 8
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 10.10.2023
Sprache Englisch
Identifikator ISSN: 0897-4756, 1520-5002
KITopen-ID: 1000163139
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Chemistry of Materials
Verlag American Chemical Society (ACS)
Band 35
Heft 19
Seiten 8065–8080
Vorab online veröffentlicht am 25.09.2023
Schlagwörter Electrodes, Materials, Polarization, Sodium, Transition metals
Nachgewiesen in Dimensions
Scopus
Web of Science
Globale Ziele für nachhaltige Entwicklung Ziel 7 – Bezahlbare und saubere Energie
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