Amorphous coordination polymers for versatile Mg<sup>2+</sup>, Ca<sup>2+</sup>, Sr<sup>2+</sup>, Ba<sup>2+</sup>, and Zn<sup>2+</sup> cation storage
Divalent metal-ion batteries hold immense promise for electrochemical energy storage applications, offering advantages in terms of volumetric capacity, cost-efficiency, sustainability, and safety. Despite advances, the lack of high-voltage and high-performance positive electrode materials remains a critical obstacle. Here, we disclose a family of amorphous coordination polymers capable of reversibly storing Mg<sup>2+</sup>, Ca<sup>2+</sup>, Sr<sup>2+</sup>, Ba<sup>2+</sup>, and Zn<sup>2+</sup> cations. For Ca<sup>2+</sup> and Mg<sup>2+</sup> systems, the highest reported working potentials of >3.2 V <i>vs.</i> Ca<sup>2+</sup>/Ca and 2.8 V <i>vs.</i> Mg<sup>2+</sup>/Mg are measured, along with fast, stable, and low-hysteresis storage without solvent or ion pair storage. These characteristics stem from the amorphous structure, delocalized anionic charge, and disordered, long bond-distance coordination, enabling weak binding and fast cation diffusion. Using sustainable elements and demonstrating universal divalent cation storage capacity by achieving the first-ever reversible storage of Sr<sup>2+</sup> and Ba<sup>2+</sup> ions, this work establishes key design principles for divalent cation storage materials and systems.
Authors
- Darsi Rambabu (ORCID: https://orcid.org/0000-0001-5771-4301)
- Petru Apostol (ORCID: https://orcid.org/0009-0005-3123-6029)
- Jan Bitenc (ORCID: https://orcid.org/0000-0002-0109-8121)
- Alexandru Vlad (ORCID: https://orcid.org/0000-0002-0059-9119)
- Koen Robeyns (ORCID: https://orcid.org/0000-0002-4763-4217)
- Jiande Wang (ORCID: https://orcid.org/0000-0003-4969-9812)
- Mengyuan Du
- Laura Simonelli (ORCID: https://orcid.org/0000-0001-5331-0633)
- Da Tie (ORCID: https://orcid.org/0009-0000-3244-9695)
- Olivera Lužanin (ORCID: https://orcid.org/0000-0002-7926-7626)
- Ashley P. Black (ORCID: https://orcid.org/0000-0001-7929-5144)
- Alexandre Ponrouch (ORCID: https://orcid.org/0000-0002-8232-6324)
- Tjaša Pavčnik (ORCID: https://orcid.org/0000-0001-7577-499X)
- Robert Markowski (ORCID: https://orcid.org/0009-0002-1150-7408)
- Jean‐François Gohy (ORCID: https://orcid.org/0000-0003-4169-1883)
- Vasudeva Rao Bakuru (ORCID: https://orcid.org/0000-0003-2582-6282)
- Xiaodong Lin (ORCID: https://orcid.org/0000-0002-1867-4789)
- Damien Monti (ORCID: https://orcid.org/0000-0002-8937-2518)
- Xiaolong Guo (ORCID: https://orcid.org/0000-0001-8636-1605)
- Raphaël Delogne
Institutions
- Centre National de la Recherche Scientifique (FR)
- ALBA Synchrotron (Spain) (ES)
- Réseau sur le Stockage Electrochimique de l'énergie (FR)
- Institut de Ciència de Materials de Barcelona (ES)
- National Institute of Chemistry (SI)
- UCLouvain (BE)
Publication Details
- Journal
- Energy & Environmental Science
- Published
- 2025-01-01
- DOI
- https://doi.org/10.1039/d5ee02567b
- Citations
- 2
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 1.46
Funders
- European Commission
- Fonds De La Recherche Scientifique - FNRS
- Fonds Wetenschappelijk Onderzoek
- China Scholarship Council
- H2020 Marie Skłodowska-Curie Actions