Metallicity, Atomic Disorder, and Li-Ion Storage in Fast-Charging Anodes
Oxides of Nb with Wadsley-Roth shear structures comprise a family of stable, high-rate anode materials for Li-ion batteries. A particular pair of them offers the unusual opportunity to test how important metallic conduction of the starting electrode is for electrode performance. The selected pair of compounds with similar 4 × 3 Wadsley-Roth block structures are insulating Ti<sub>2</sub>Nb<sub>10</sub>O<sub>29</sub> and metallic Nb<sub>12</sub>O<sub>29</sub>. A combination of diffraction, electrochemistry, magnetic measurements, and entropic potential measurements is employed to establish key findings for these two anode materials. We find that starting with a metallic oxide is not especially advantageous over a comparable material that readily transitions into a metallic state upon lithiation. Second, the rate performance appears to be dictated by ion mobility, and atomic Ti/Nb disorder in Ti<sub>2</sub>Nb<sub>10</sub>O<sub>29</sub> contributes to improved capacity retention at high rates by suppressing Li-ion ordering. However, subtle details in the nature of redox processes make Nb<sub>12</sub>O<sub>29</sub> a slightly better electrode material for long-term cycling at slower rates.
Authors
- Ram Seshadri (ORCID: https://orcid.org/0000-0001-5858-4027)
- Ashlea Patterson (ORCID: https://orcid.org/0000-0002-0458-4029)
- Linus Kautzsch (ORCID: https://orcid.org/0000-0003-1999-436X)
- Krishna Prasad Koirala (ORCID: https://orcid.org/0000-0002-9137-917X)
- Anna Kallistová (ORCID: https://orcid.org/0000-0003-1320-0071)
- Wenqian Xu (ORCID: https://orcid.org/0000-0002-4815-6253)
- Laurent Pilon (ORCID: https://orcid.org/0000-0001-9459-8207)
- Arava Zohar (ORCID: https://orcid.org/0000-0002-8292-5968)
- Kira E. Wyckoff (ORCID: https://orcid.org/0000-0003-4353-9447)
- Anthony K. Cheetham (ORCID: https://orcid.org/0000-0003-1518-4845)
- H. Cein Mandujano (ORCID: https://orcid.org/0000-0003-2073-7061)
- Welton Wang
- Tianyu Li (ORCID: https://orcid.org/0000-0003-0142-7252)
- Jue Liu (ORCID: https://orcid.org/0000-0002-4453-910X)
- Yucheng Zhou (ORCID: https://orcid.org/0000-0002-7436-4451)
- Ananya Kepper
Institutions
- Argonne National Laboratory (US)
- Oak Ridge National Laboratory (US)
- University of California, Santa Barbara (US)
- University of California System (US)
- Samueli Institute (US)
- Advanced Photonix (United States) (US)
- Advanced Photon Source
- University of Maryland, College Park (US)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-09-02
- DOI
- https://doi.org/10.1021/jacs.5c06578
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Basic Energy Sciences