Wang, K;
Chu, Y;
Huang, Z;
Yang, H;
Yang, M;
Mu, Y;
Tan, X;
... Hu, J; + view all
(2025)
Unleashing the Kinetic Limitation of Co-Free Li-Rich Mn-Based Cathodes via Ionic/Electronic Dual-Regulation.
Advanced Materials
, Article 2504642. 10.1002/adma.202504642.
(In press).
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Abstract
Li-rich Mn-based oxide (LRMO) are promising cathode candidates for next-generation Li-ion batteries with combined cost-effectiveness and high specific capacity. Designing Co-free LRMO can further leverage the low cost of this class of cathodes given the capacity can be maintained. However, implementing cobalt-free LRMO cathode materials are hampered by their sluggish kinetics, resulting in low capacity and poor rate performance that underperform compared with their Co-containing counterparts. Here, it is confirmed that the slow kinetics of Co-free LRMO originates from the structural disorder caused by transition metals (TMs) migration at high voltages (above 4.5 V Vs. Li+/Li) and consequent irreversible oxygen redox process. Aware of this, Na+/F− is introduced in surficial lattice to alleviate these issues, ultimately achieving improved discharge voltage (≈0.2 V above 1 C, 1 C = 0.25 A g−1), exceptional cycle stability in pouch-type cell (95.1% capacity retention in 1 C after 400 cycles at 25 °C, and 80.9% capacity retention after 300 cycles in 0.5 C at 45 °C) and excellent C-rate performance (≈150 mA h g−1 at 5 C). The newly developed Na+/F− gradient design unleashes the surficial charge transfer kinetics limitation and greatly improves the lattice structure stability, consequently providing valuable guidelines for future high-capacity LRMO cathode design.
| Type: | Article |
|---|---|
| Title: | Unleashing the Kinetic Limitation of Co-Free Li-Rich Mn-Based Cathodes via Ionic/Electronic Dual-Regulation |
| Location: | Germany |
| DOI: | 10.1002/adma.202504642 |
| Publisher version: | https://doi.org/10.1002/adma.202504642 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Gradient doping; high electrochemical performance; ionic/eletronic regulation; Li-rich Co-free cathode |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10210703 |
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