2D-on-2D Al-Doped NiCo LDH Nanosheet Arrays for Fabricating High-Energy-Density, Wide Voltage Window, and Ultralong-Lifespan Supercapacitors.

Battery-type electrode materials with high capacity, wide potential windows, and good cyclic stability are crucial to breaking through energy storage limitations and achieving high energy density. Herein, a novel 2D-on-2D Al-doped NiCo layered double hydroxide (NiCoAlx LDH) nanosheet arrays with high-mass-loading are grown on a carbon cloth (CC) substrate via a two-step hydro/solvothermal deposition strategy, and the effect of Al doping is employed to modify the deposition behavior, hierarchical morphology, phase stability, and multi-metallic synergistic effect. The optimized NiCoAl0.1 LDH electrode exhibits capacities of 5.43, 6.52, and 7.25 C cm-2 (9.87, 10.88, and 11.15 F cm-2) under 0-0.55, 0-0.60, and 0-0.65 V potential windows, respectively, illustrating clearly the importance of the wide potential window. The differentiated deposition strategy reduces the leaching level of Al3+ cations in alkaline solutions, ensuring excellent cyclic performance (108% capacity retention after 40 000 cycles). The as-assembled NiCoAl0.1 LDH//activated carbon cloth (ACC) hybrid supercapacitor delivers 3.11 C cm-2 at 0-2.0 V, a large energy density of 0.84 mWh cm-2 at a power density of 10.00 mW cm-2, and excellent cyclic stability with ≈135% capacity retention after 150 000 cycles.

Quasi-Parallel NiFe Layered Double Hydroxide Nanosheet Arrays for Large-Current-Density Oxygen Evolution Electrocatalysis.

Designing advanced electrocatalysts for oxygen evolution at large current density (>500 mA cm-2 ) is critical to practical water splitting applications. Herein, a novel quasi-parallel NiFe layered double hydroxide (NiFe LDH) nanosheet arrays with pattern alignment on Ni foam was developed. The initial α-Ni(OH)2 layer induced effective coprecipitation between Ni2+ and Fe3+ for the formation of LDH phase, guaranteeing the electronic pulling effect among metal cations and enhancing the interaction between active materials and substrate for excellent adhesion and electrical conductivity. Quasi-parallel NiFe LDH nanoarrays exhibited outstanding oxygen evolution activity with a small Tafel slope of 30.1 mV dec-1 and overpotentials of 196, 255, and 284 mV at a current density of 10, 500, and 1000 mA cm-2 in 1.0 m KOH solution, respectively, and high stability over 40 h at 750 mA cm-2 . This work presents a new strategy towards fabricating electrode materials with exceptional performance.