Abstract

Optimized porous structure is a prerequisite for high performance Li‒O2 battery cathode. Macroporous-mesoporous carbon (MMC) is fabricated via a nano-replication method using mesoporous SiO2 (KIT-6) containing NiO as the template. By varying the amount of NiO in the KIT-6/NiO composite template, the amount of macropores inside MMC is easily controlled. The as-prepared MMC exhibits a highly porous structure with abundant ordered mesopores along with macropores that are larger than 200 nm in size. When the MMC is applied as the cathode material in a Li‒O2 battery, the cell exhibits greatly improved electrochemical performance in comparison to a cell using conventional ordered mesoporous carbon (OMC) without macropores. Systematic studies indicate that while mesopores in the OMC are clogged with Li2O2 formed during the early stage of discharge, the MMC sufficiently accommodates a large amount of Li2O2 in the pores. In addition, Li2O2 with poor crystallinity forms on the cathode containing MMC during subsequent discharge processes, which can be due to the accumulated side product and the limited size of pores. The formation of amorphous Li2O2 and the expedited mass transport through the interconnected meso- and macropores of MMC can attribute to the improved electrochemical performance of the MMC cathode material.

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