He, Shunli;
Young, Robert Scott;
Shen, Xing;
Han, Miao;
Song, Yaoguang;
Dong, Wenyi;
Zhang, Yiming;
... Rettie, Alexander JE; + view all
(2025)
Ionic-Potential-Guided Fluoride Engineering of Reversible Mn-Based Cathodes for Sodium-Ion Batteries.
ACS Nano
, 19
(39)
, Article acsnano.5c10781. 10.1021/acsnano.5c10781.
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Text (Accepted Manuscript)
Shunli_Ionic-Potential-Guided Fluoride Engineering of Reversible Mn-Based Cathodes for Sodium-Ion Batteries_AAM.pdf - Accepted Version Access restricted to UCL open access staff until 27 September 2026. Download (3MB) |
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Text (Supplementary Material)
Shunli_Ionic-Potential-Guided Fluoride Engineering of Reversible Mn-Based Cathodes for Sodium-Ion Batteries_SuppM.pdf - Accepted Version Access restricted to UCL open access staff until 27 September 2026. Download (4MB) |
Abstract
Mn-based layered oxides are promising cathode materials for sodium-ion batteries (SIBs) due to their high capacity and cost-effectiveness. However, their practical application is often hindered by structural instability and Jahn-Teller distortion associated with Mn3+. Herein, an ionic-potential-guided metal-fluoride engineering strategy is proposed to address these challenges by coincorporating AlF3 with transition-metal vacancies into a P2-type Mn-based layered oxide (Na0.76Ni0.225Al0.0167Mn0.75O1.95F0.05). This dual-site tuning elevates total ionic potential from 15.37 to 15.61 by simultaneously enhancing the cationic potential and reducing the anionic contribution, thereby promoting interlayer stability and suppressing Jahn-Teller effects. Multiscale characterization and density functional theory calculations reveal a reversible, solid-solution Na+ (de)intercalation mechanism with a negligible lattice strain (∼0.15%) and suppressed Mn3+ formation. The optimized cathode delivers an average voltage of ≈3.60 V within 2.0 to 4.3 V range, a reversible capacity of 134 mA h g-1, and 83% capacity retention after 100 cycles (2.0-4.3 V, 1C). In contrast, the pristine counterpart shows a lower average voltage of 3.32 V and a rapid capacity drop to ∼50 mA h g-1 by the second cycle. These findings establish the ionic-potential-guided AlF3 incorporation as a robust and scalable strategy for designing highly reversible, high-voltage, and long-life cathodes for next-generation SIBs.
| Type: | Article |
|---|---|
| Title: | Ionic-Potential-Guided Fluoride Engineering of Reversible Mn-Based Cathodes for Sodium-Ion Batteries |
| Location: | United States |
| DOI: | 10.1021/acsnano.5c10781 |
| Publisher version: | https://doi.org/10.1021/acsnano.5c10781 |
| 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: | high voltage, ionic-potential engineering, metal-fluoride doping, P2-type Mn-based layered cathodes, reversible cation/anion redox, sodium-ion batteries |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Engineering Science Faculty Office |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10215700 |
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