Boosting the sodium storage performance of iron selenides by a synergetic effect of vacancy engineering and spatial...

Recently, iron selenides have been considered as one of the most promising candidates for the anodes of sodium-ion batteries (SIBs) due to their cost-effectiveness and high theoretical capacity; however, their practical application is limited by poor conductivity, large volume variation and slow reaction kinetics during electrochemical reactions. In this work, spatially dual-carbon-confined V_Se-Fe₃Se_4-xS_x/FeSe_2-xS_x nanohybrids with abundant Se vacancies (V_Se-Fe₃Se_4-xS_x/FeSe_2-xS_x@NSC@rGO) are constructed via anion doping and carbon confinement engineering. The three-dimensional crosslinked carbon network composed of the nitrogen-doped carbon support derived from polyacrylic acid (PAA) and reduced graphene enhances the electronic conductivity, provides abundant channels for ion/electron transfer, ensures the structure integrity, and alleviates the agglomeration, pulverization and volume change of active material during the chemical reactions. Moreover, the introduction of S into iron selenides induces a large number of Se vacancies and regulates the electron density around iron atoms, synergistically improving the conductivity of the material and reducing the Na⁺ diffusion barrier. Based on the aforementioned features, the as-synthesized V_Se-Fe₃Se_4-xS_x/FeSe_2-xS_x@NSC@rGO electrode possesses excellent electrochemical properties, exhibiting the satisfactory specific capacity of 630.1 mA h g^-1 after 160 cycles at 0.5 A/g and the reversible capacity of 319.8 mA h g^-1 after 500 cycles at 3 A/g with the low-capacity attenuation of 0.016 % per cycle. This investigation provides a feasible approach to develop high-performance anodes for SIBs via a synergetic strategy of vacancy engineering and carbon confinement.