Facile fabrication of Ni, Fe-doped δ-MnO2 derived from Prussian blue analogues as an efficient catalyst for stable Li-CO2 batteries.

ABSTRACT

Rechargeable Li-CO2 batteries are regarded as an ideal new-generation energy storage system, owing to their high energy density and extraordinary CO2 capture capability. Developing a suitable cathode to improve the electrochemical performance of Li-CO2 batteries has always been a research hotspot. Herein, Ni-Fe-δ-MnO2 nano-flower composites are designed and synthesized by in situ etching a Ni-Fe PBA precursor as the cathode for Li-CO2 batteries. Ni-Fe-δ-MnO2 nanoflowers composed of ultra-thin nanosheets possess considerable surface spaces, which can not only provide abundant catalytic active sites, but also facilitate the nucleation of discharge products and promote the CO2 reduction reaction. On the one hand, the introduction of Ni and Fe elements can improve the electrical conductivity of δ-MnO2. On the other hand, the synergistic catalytic effect between Ni, Fe elements and δ-MnO2 will greatly enhance the cycling performance and reduce the overpotential of Li-CO2 batteries. Consequently, the Li-CO2 battery based on the Ni-Fe-δ-MnO2 cathode shows a high discharge capacity of 8287 mA h g-1 and can stabilize over 100 cycles at a current density of 100 mA g-1. The work offers a promising guideline to design efficient manganese-based catalysts for Li-CO2 batteries.