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Alternative Polymorph of the Hydroxysulfate Li x FeSO 4 OH Yields Improved Lithium-Ion Cathodes

Singh, Shashwat; Chakraborty, Arup; Neveu, Audric; Jha, Pawan Kumar; Pralong, Valérie; Fichtner, Maximilian 1,2; Islam, M. Saiful ; Barpanda, Prabeer 1
1 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)
2 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

Use of sustainable electrode components in Li-ion battery technology is essential for large-scale applications while addressing environmental concerns. Considering elemental abundance, Fe-based compounds can, in principle, work as the most economic cathodes. Fe-based hydroxysulfates LixFeSO$_4$OH (x = 0 –1) can be harnessed as low-cost, sustainable, high-voltage, and moisture-resistant battery cathode materials. In this system, monoclinic (m) FeSO$_4$OH and layered m-FeSO4OH were previously reported as Li-ion battery cathode materials. Here, we introduce orthorhombic (o) FeSO4OH as a potential low-cost cathode for Li-ion batteries synthesized by using a facile low-temperature hydrothermal route. The o-FeSO$_4$OH cathode delivers a reversible capacity of 100 mA h/g at a current rate of C/20 (1e– = 159 mAh/g) at a working potential of ca. 3.2 V vs Li$^+$/Li. A higher overpotential and faster rate kinetics compared with that of m-FeSO4OH stem from the subtle deviations in the structural framework affecting the Li coordination environment. Operando analytical tools, electrochemical titration techniques, and computational modeling are combined to characterize the complex phase transformation during the (de)lithiation process.


Verlagsausgabe §
DOI: 10.5445/IR/1000173831
Veröffentlicht am 30.08.2024
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Institut für Nanotechnologie (INT)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2024
Sprache Englisch
Identifikator ISSN: 0897-4756, 1520-5002
KITopen-ID: 1000173831
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Chemistry of Materials
Verlag American Chemical Society (ACS)
Band 36
Heft 16
Seiten 8088-8097
Vorab online veröffentlicht am 14.08.2024
Nachgewiesen in Web of Science
Dimensions
Scopus
Globale Ziele für nachhaltige Entwicklung Ziel 7 – Bezahlbare und saubere Energie
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