Abstract

Sodium-ion hybrid capacitors (SIHCs) are desirable energy storage devices due to the combined advantages of their battery- and capacitive-type electrodes. However, their further development is mainly handicapped by the battery-type electrodes, which suffer from poor cycling stabilities and rate capacities caused by dramatic volume changes and Na+ ion's intrinsically sluggish diffusion, respectively. Hence, we synthesized a Ni-based framework encapsulated with graphene oxide (Ni-MOF@GO) composites containing hexa(4-carboxyl-phenoxy)-cyclotriphosphazene (HCTP-COOH) ligands. The reported one-step selenization of Ni-MOF@GO composites realizes the space-confined growth of ultrafine nickel selenide wrapped in a multi-heteroatom-doped carbon matrix (NiSe@C/rGO). The synergic combination of downsizing, carbon encapsulation, and multi-heteroatom doping strategy on the specific NiSe@C/rGO composites improves cycling stability and superior rate performance for sodium-ion storage. The NiSe@C/rGO electrode displays a high specific capacity of 448.9 mAh g−1 at 0.1 A g−1, excellent rate capability with 272.3 mAh g−1 at 10 A g−1, and a remaining capacity of 263.9 mAh g−1 with 1000 testing cycles at 1.0 A g−1. In addition, the battery-type electrode NiSe@C/rGO with improved rate capacity and cycling stability enables an optimal SIHC delivering a maximum energy density of 60.5 Wh kg−1, a power density of 13,340 W kg−1 at 37 Wh kg−1, and capacity retention of 75% after 5000 cycles at 2.0 A g−1.

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