4.8 Article

Resolving the Incomplete Charging Behavior of Redox-Mediated Li-O2 Batteries via Sustainable Protection of Li Metal Anode

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c14349

Keywords

lithium-oxygen batteries; lithium metal protection; artificial protection layer; redox mediator; incomplete charging behavior

Funding

  1. Human Resources Development program of a Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant - Ministry of Trade, Industry and Energy of the Korean government [20214000000320]
  2. National Research Foundation of Korea (NRF) grant - Korean government Ministry of Education and Science Technology (MEST) [NRF-2018R1A2B3008794]

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This study explores the incomplete charging behavior of lithium-oxygen batteries (LOBs) operated at a feasible capacity and proposes a lithium protection strategy to improve their rechargeability. The research provides guidelines for achieving sustainable cycling of LOBs and offers a feasible approach for the practical use of high areal capacity LOBs.
Lithium-oxygen batteries (LOBs) have attracted worldwide attention due to their high specific energy. However, the poor rechargeability and cycling stability of LOBs hinders their practical use in applications. Here, we explore the incomplete charging behavior of redox-mediated LOBs operated at a feasible capacity for a practical level (3.25 mAh cm-2) and resolve it using a sustainable lithium protection strategy. The incomplete charging behavior, promoted by self-discharge of redox mediators (RMs), hampers the reversible cycling of LOBs, which was investigated through multiangle in situ and ex situ analyses. Meanwhile, the proposed lithium protection strategy, introducing an inorganic/ organic hybrid artificial composite layer with a preformed stable interface between the lithium metal and the composite layer, enhances the stability of the lithium metal anode during the prolonged cycling by preventing the chemical/electrochemical interactions of RMs on the lithium metal surface, thus improving the overall rechargeability of LOBs. This work provides guidelines for the effective use of RMs with an adequate lithium protection strategy to achieve sustainable cycling of LOBs, creating a feasible approach for the practical use of LOBs with high areal capacity.

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