Abstract

Lithium‐air battery has emerged as a viable electrochemical energy technology; yet a substantial overpotential is typically observed, due to the insulating nature of the discharge product Li2O2 that hinders the reaction kinetics and device performance. Furthermore, finite solid–solid/–liquid interfaces are formed between Li2O2 and catalysts and limit the activity of the electrocatalysts in battery reactions, leading to inadequate electrolytic efficiency. Herein, in‐situ doping of Li2O2 by select metal ions is found to significantly enhance the lithium‐air battery performance, and Co2+ stands out as the most effective dopant among the series. This is ascribed to the unique catalytic activity of the resulting Co‐Ox sites towards oxygen electrocatalysis, rendering the lithium‐air battery self‐catalytically active. Theoretical studies based on density functional theory calculations show that structural compression occurs upon Co2+ doping, which lowers the energy barrier of Li2O2 decomposition. Results from this study highlight the significance of in situ electrochemical doping of the discharge product in enhancing the performance of lithium‐air battery.

Highlights

  • With the development of electrical vehicles, the demand for effective energy conversion and storage technologies has never been higher,[1,2,3,4] as conventional lithium-ion battery is approaching its theoretical limit (500 Wh kg-1) for the emerging energy market.[5, 6] Lithium-air battery (LAB) represents a promising alternative, exhibiting a remarkable theoretical energy density of 11,400 Wh kg-1.[7]

  • Yet it suffers from a low round-trip efficiency and poor cyclability, mainly due to the sluggish reaction kinetics.[8, 9]

  • By combining density functional theory (DFT) calculations and experimental results obtained above, we propose a mechanism for the enhanced performance of self-catalyzed LAB (SCLAB) (Figure 5j)

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Summary

UC Irvine Previously Published Works

Title Self‐Catalyzed Rechargeable Lithium‐Air Battery by in‐situ Metal Ion Doping of Discharge Products: A Combined Theoretical and Experimental Study.

Accepted Article
Introduction
Results and Discussion
Conclusion
Table of content

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