Abstract
The sluggish oxygen reaction kinetics concomitant with the high overpotentials and parasitic reactions from cathodes and solvents is the major challenge in aprotic lithium-oxygen (Li–O2) batteries. Herein, PtIr multipods with a low Lewis acidity of the Pt atoms are reported as an advanced cathode for improving overpotentials and stabilities. DFT calculations disclose that electrons have a strong disposition to transfer from Ir to Pt, since Pt has a higher electronegativity than Ir, resulting in a lower Lewis acidity of the Pt atoms than that on the pure Pt surface. The low Lewis acidity of Pt atoms on the PtIr surface entails a high electron density and a down-shifting of the d-band center, thereby weakening the binding energy towards intermediates (LiO2), which is the key in achieving low oxygen-reduction-reaction (ORR) and oxygen-evolution-reaction (OER) overpotentials. The Li–O2 cell based on PtIr electrodes exhibits a very low overall discharge/charge overpotential (0.44 V) and an excellent cycle life (180 cycles), outperforming the bulk of reported noble-metal-based cathodes.
| Original language | English |
|---|---|
| Pages (from-to) | 26592-26598 |
| Number of pages | 7 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 60 |
| Issue number | 51 |
| DOIs | |
| Publication status | Published - 13 Dec 2021 |
Keywords
- Lewis acidity
- PtIr multipods
- adsorption energy
- lithium–oxygen batteries
- overpotentials
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