Unveiling the mechanism and interactions happening in cobalt selenide cathode for Rechargeable aluminium batteries

Eliana Fuentes-Mendoza^a, Angelina Sarapulova^b^,^c, Ramon Zimmermanns^a, Eugen Zemlyanushin^a, Fabian Jeschull^a, Sonia Dsoke^b^,^c^,^d

^aKarlsruhe Institute of Technology (KIT), Karlsruhe, Engesserstr. 13, 76131, Germany, Engesserstrasse 13, Gebaude 30.34, Karlsruhe, Germany

^bFraunhofer Institute for Solar Energy Systems ISE, Freiburg, Germany

^cFreiburg Materials Research Center FMF, University of Freiburg, Stefan-Meier-Straße 21, 79104 Freiburg, Germany

^dUniversity of Freiburg, Institute for Sustainable Systems Engineering (INATECH)

Proceedings of MATSUS Fall 2025 Conference (MATSUSFall25)

C1 Emerging sustainable battery technologies: advances in electrode, electrolyte and interf(ph)ase design - #SusBat

València, Spain, 2025 October 20th - 24th

Organizers: Nuria Tapia Ruiz and Maider Zarrabeitia

Oral, Eliana Fuentes-Mendoza, presentation 142
Publication date: 21st July 2025

In recent years, sustainable battery systems based on Na, Ca, Al, Cl, and Mg have been studied as a complement to Li-ion batteries. Theoretically, the use of aluminum as the negative electrode would bring some important advantages, such as high theoretical specific gravimetric and volumetric capacities, comparable to those of lithium-based systems. However, this emerging technology presents challenges due to the high corrosivity of the commonly used non-aqueous electrolyte AlCl₃/(EMIm)Cl [1-2].

The latest research on cathodes for aluminum batteries includes carbon-, metal oxides-, and metal chalcogenide-based materials. Carbon-based materials have shown excellent cycling stability and their mechanism is based on the insertion and disinsertion of chloroaluminate anions ([AlCl₄]^- and [Al₂Cl₇]^-). Metal chalcogenides have been studied widely. Specifically, in cobalt selenide, it is believed that the high polarizable Al-Se/S bond allows the insertion/extraction of Al³⁺ and takes advantage of the three-electron redox reaction. [2-3]

In this work, we have examined cobalt selenide via in-situ and -operando XRD to determine the interactions happening at the material during the first cycle, combined with a series of electrochemical and ex-situ characterizations and this way unveil the energy storage and degradation mechanism of CoSe. The results indicate that during the first cycle, CoSe undergoes a phase transition to CoSe₂, accompanied by structural disorder and a loss of long-range crystallinity. This transformation impacts cycling stability causing cobalt dissolution and migration to the aluminum anode. Understanding the cathode processes during cycling could guide the development of high-energy-density, high-power, and stable electrodes for aluminum batteries.

References:

[1] Xing, S. W., & Yan, Z. (2018). Stable CoSe2/Carbon Nanodice@Reduced Graphene Oxide Composites for High-Performance Rechargeable Aluminum-ion Batteries. Energy Environ. Sci, 11, 2341.

[2] Zhou, Q., Zheng, Y., Wang, D., Lian, Y., Ban, C., Zhao, J., & Zhang, H. (2020). Cathode Materials in non-Aqueous Aluminum-ion Batteries: Progress and Challenges. In Ceramics International (Vol. 46, Issue 17, pp. 26454–26465). Elsevier Ltd.

[3] Zafar, Z. A., Imtiaz, S., Razaq, R., Ji, S., Huang, T., Zhang, Z., Huang, Y., & Anderson, J. A. (2017). Cathode Materials for Rechargeable Aluminum Batteries: Current Status and Progress. In Journal of Materials Chemistry A (Vol. 5, Issue 12, pp. 5646–5660). Royal Society of Chemistry.

Acknowledgements:

This work contributes to the research performed at CELEST (Center for Electrochemical Energy Storage Ulm-Karlsruhe) and was funded by the German Research Foundation (DFG) under Project ID 390874152 (POLiS Cluster of Excellence).

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