Achieving Ultrafast and Stable Na-Ion Storage in FeSe2 Nanorods/Graphene Anodes by Controlling the Surface Oxide

Designing transitional metal selenides (TMSes) with superior rate and cyclic performance for sodium-ion storage remains great challenges. To achieve this task, the influence of surface oxides on Na-ion storage behavior of FeSe2 is investigated by designing FeSe, with varying oxide content. It is found that surface oxide has an inhibitory effect on the activity of FeSe2. Small-sized FeSe, on graphene with higher surface oxide content exhibits obviously inferior performance compared to large-sized FeSe2 with lower oxide content. By controlling oxide content, the prepared FeSe2 nanorods/graphene exhibits a high capacity of 459 mAh/g at 0.1 A/g and superior rate performance. Only 10% capacity decrease occurs with the increase in current density from 0.1 to 5 A/g. Even at 25 A/g (similar to 50 C), it delivers a capacity of 227 mAh/g with almost no decay after 800 cycles. The influence mechanism of surface oxide is investigated. The oxide can be converted to a sodiated shell with high mechanical strength and poor conductivity, which generates phase-transition resistance to suppress the sodiation of FeSe2 core, blocks the transfer of Na-ions and electrons in subsequent sodiation processes. Understanding the effect of surface oxide on Na-ion storage will be helpful in designing TMSes and other active materials.