LAUSR

Transition metal phosphides (TMPs) possess high theoretical sodium storage capacities, but suffer from poor rate performance, due to their intrinsic low conductivity and large volume expansion upon sodiation/desodiation. Compositing TMPs with carbon materials or downsizing their feature size are recognized as efficient approaches to address the above issues. Nevertheless the surface‐controlled capacitive behavior is generally dominated, which inevitably compromises the charge/discharge platform, and decreases the operational potential window in full‐cell constructions. In this work, a novel architecture (FeP@OCF) with FeP quantum dots confined in P‐doped 3D octahedral carbon framework/carbon nanotube is rationally designed. Such structure enables a simultaneous enhancement on the diffusion‐controlled capacity in the platform region (2.3 folds), and the surface‐controlled capacity in the slope region (2.9 folds) as compared to that of pure FeP. As a result, an excellent reversible capacity (674 mAh g−1@ 0.1 A g−1) and a record high‐rate performance (262 mAh g−1 @ 20 A g−1) are achieved. A full‐cell FeP@OCF// Na3V2(PO4)3 is also constructed showing an outstandingly high energy density of 185 Wh kg−1 (based on the total mass of active materials in both electrodes), which outperforms the state‐of‐the art TMP‐based sodium‐ion battery full cells.