Controlled establishment of advanced local high-entropy NiCoMnFe-based layered double hydroxide for zinc batteries and low-temperature supercapacitors

The development of high-performance electrodes is essential for improving the charge storage performance of rechargeable devices. In this study, local high-entropy C, N co-doped NiCoMnFe-based layered double hydroxide (C/N-NiCoMnFe-LDH, C/N-NCMF) were designed using a novel method. Multi-component synergistic effects can dramatically modulate the surface electron density, crystalline structure, and band-gap of the electrode. Thus, the electrical conductivity, electron transfer, and affinity for the electrolyte can be optimized. Additionally, the C/N-NCMF yielded a high specific capacitance (1454F·g−1) at 1 A·g−1. The electrode also exhibited excellent cycling stability, with 62 % capacitance retention after 5000 cycles. Moreover, the assembled Zn||C/N-NCMF battery and the C/N-NCMF//AC hybrid supercapacitor yielded excellent energy densities of 63.1 and 35.4 Wh·kg−1 at power densities of 1000 and 825 W·kg−1, and superior cycling performance with 69 % and 88.7 % capacitance retention after 1000 and 30,000 cycles, respectively. Furthermore, the electrode maintained high electrochemical activity and stability and ensured high energy density, power density, and cycling stability of the rechargeable devices even at a low temperature (−20 °C). This study paves a new pathway for regulating the electrochemical performance of LDH-based electrodes.