Sulfur and phosphorus co-doped nickel–cobalt layered double hydroxides for enhancing electrochemical reactivity and supercapacitor performance

Abstract

Layered double hydroxides (LDHs) have drawn significant interest as emerging active materials for advanced energy storage devices; however, their low electric and ionic conductivity limit their applications. In this study, we report sulfur (S) and phosphorus (P) co-doped NiCo LDH nanoarrays prepared via a facile phosphor–sulfurization process to impart diverse co-doping effects. Combining the benefits of their unique hierarchical structure and reduced charge transfer resistance, the S and P co-doped NiCo LDH (NiCo LDH-SP) nanoarrays realize faster and more efficient redox reactions and achieve enhanced surface reactivity, thereby resulting in a performance superior to that of pristine NiCo LDH. Therefore, a NiCo LDH-SP shows an ultra-high specific capacitance of 3844.8 F g⁻¹ at a current density of 3 A g⁻¹ and maintains a specific capacitance of 2538.8 F g⁻¹ at a high current density of 20 A g⁻¹. Additionally, an asymmetric supercapacitor, assembled with the NiCo LDH-SP as the cathode and activated carbon (AC) as the anode (NiCo LDH-SP//AC), shows a high energy density of 74.5 W h kg⁻¹ at a power density of 0.8 kW kg⁻¹ and outstanding cycling stability, thereby retaining ∼81.3% of its initial specific capacitance after 5000 cycles. This study presents a facile and promising strategy for developing LDH-based electrode materials with excellent electrochemical performance for advanced energy storage applications.