Surface engineering donor and acceptor sites with enhanced charge transport for low-overpotential lithium–oxygen batteries

Inferior charge transport in discharge products is one of the main factors restricting the technological potential of lithium-oxygen batteries. Here, we propose a strategy to enhance charge transport in discharge products by surface engineering of cathode catalysts with donor and acceptor sites to improve solid-solid interfacial electron transfer properties between catalysts and discharge products. Free-standing layered double oxides loaded with pyrolyzed sodium poly(aminobenzenesulfonate)-derived sulfur-doped carbon nanosheets and carbon nanosheets with sulfoxide groups are synthesized and utilized to investigate donor and acceptor sites effect on the performance of lithium-oxygen batteries. The free-standing cathode with hybrid donor and acceptor sites is capable of operation in oxygen with distinct (dis)charge plateau and superior cycling stability (over 60 cycles at a fixed capacity of 0.53 mAh cm−2). The superior properties are attributed to the enhanced charge transport in lithium peroxide by the formation of hole polarons/Li+ vacancies on acceptor sites and electron polarons/disordered lithium peroxide phase on donor sites. This work provides a promising route to enhance defective charge transport in discharge products by optimization of donor and acceptor sites on cathode catalysts for high-performance lithium-oxygen batteries.