Dual-Carbon Engineering of Nanosized (Ni_0.28Co_0.72)_1–xS for Li⁺ Storage with Enhanced Rate Capability and Stability

Abstract

The poor conductivity and large volume swelling of transition-metal sulfides are still big challenges to overcome for highperformance energy storage. Herein, the flexibility of MOF precursors offers remarkable versatility in tailoring the chemical composition of NiCo sulfides with a highly desirable porous structure, and then dualcarbon-confined (Ni 0.28 Co 0.72 ) 1−x S nanoparticles are designed, in which an inner sulfur-doped porous carbon (SC) matrix (derived from the organic ligands of metal−organic frameworks (MOFs)) and an outer wrapped S-doped reduced graphene oxide (SG)-co-engineered (Ni 0.28 Co 0.72 ) 1−x S are constructed ((Ni 0.28 Co 0.72 ) 1−x S/SC/SG)) to enhance the rate capability and stability of Li + storage. For the dual carbons, the inner SC can elastically realize the anti-aggregation of nanosized (Ni 0.28 Co 0.72 ) 1−x S and improve their conductivity, while the outer SG could further promote the reaction kinetics, stabilize the structure, and ensure the structural integrity. As expected, the optimized (Ni 0.28 Co 0.72 ) 1−x S/SC/0.7SG exhibits an outstanding rate capability of 640.1 mAh g −1 at 5.0 A g −1 and ultrahigh cycling stability of 134.7% at 1 A g −1 after 1000 cycles. The assembled lithiumion capacitor (LIC) also shows a high energy density of 125.8 Wh kg −1 at the power density of 200 W kg −1 , as well as excellent stability (98.8% after 6000 cycles). This work highlights the significance of dual-carbon engineering in enhancing the energy storage performance of active materials, and the fabricated nanosized (Ni 0.28 Co 0.72 ) 1−x S by dual-carbon engineering can be applied in highperformance electrochemical energy storage and beyond.