Defect-Engineered NiCo-S Composite as a Bifunctional Electrode for High-Performance Supercapacitor and Electrocatalysis

Defect engineering is a reasonable solution to improve the surface properties and electronic structure of nanomaterials. However, how to introduce dual defects into nanomaterials by a simple way is still facing challenge. Herein, we propose a facile two-step solvothermal method to introduce Fe dopants and S vacancies into metal-organic framework-derived bimetallic nickel cobalt sulfide composites (NiCo-S). The as-prepared Fedoped NiCo-S (Fe-NiCo-S) possesses improved charge storage kinetics and activities as electrode material for supercapacitors and the oxygen evolution reaction (OER). The obtained Fe-NiCo-S nanosheet has a high specific capacitance (2779.6 F g(-1) at 1 A g(-1)) and excellent rate performance (1627.2 F g(-1) at 10 A g(-1)). A hybrid supercapacitor device made of Fe-NiCo-S as the positive electrode and reduced graphene oxide (rGO) as the negative electrode presents a high energy density of 56.0 Wh kg(-1) at a power density of 847.1 W kg(-1) and excellent cycling stability (capacity retention of 96.5% after 10,000 cycles at 10 A g(-1)). Additionally, the Fe-NiCo-S composite modified by Fe doping and S vacancy has an ultralow oxygen evolution overpotential of 247 mV at 10 mA cm(-2). Based on the density functional theory (DFT) calculation, defects cause more electrons to appear near the Fermi level, which is conducive to electron transfer in electrochemical processes. Our work provides a rational strategy for facilely introducing dual defects into metal sulfides and may provide a novel idea to prepare electrode materials for energy storage and energy conversion application.

Automated summary

Defect engineering is a feasible approach to enhance the properties of nanomaterials, but introducing dual defects in a simple way remains a challenge. In this study, Fe-doped NiCo-S nanosheets with improved charge storage kinetics were successfully synthesized. These materials showed high specific capacitance and excellent rate performance, making them promising electrode materials for supercapacitors and the OER. The introduction of dual defects through a two-step solvothermal method provides a rational strategy for preparing high-performance electrode materials.