Encapsulation of Selenium in MOF-Derived N,O-Codoped Porous Flower-Like Carbon Host for Na-Se Batteries

Abstract Na-Se batteries have their drawbacks such as large volumetric expansion and shuttle effect related to generation of soluble sodium polyselenides. To address these issues, a nitrogen and oxygen codoped flower-like porous carbon host is derived from a Ni-based metal–organic framework (MOF) for Se storage. The use of 4,4′-oxybisbenzoic acid and 4,4′-dimethyl-2,2′-bipyridyl ligands ensure the in-situ doping of the carbon host with oxygen and nitrogen upon carbonization of MOF, which increases its polarity and restricts the diffusion of selenium. Highly porous microflower-like carbon morphology provides sufficient space for Se storage. To avoid undesirable aggregation of Se particles which happens when using conventional melt-diffusion method, we employed a vapor-infiltration method for Se loading, which ensures the homogeneous dispersion of selenium and high utilization of pores in the carbon host. Density functional theory calculations confirmed that the increased polarity of the carbon host due to N,O codoping promotes the adsorption of polyselenides. When tested as a cathode for sodium-selenium battery, the optimized carbon/selenium composite shows an excellent electrochemical performance.