Hierarchical NiMn/NiMn-LDH/ppy-C induced by a novel phase-transformation activation process for long-life supercapacitor

For micron-sized nickel-based hydroxides sheets, the reaction and migration of anions/water molecules in the inner region tends to lag behind those along the edge, which can cause structure mismatch and capacity degradation during cycles. Nanosizing and structure design is a feasible solution to shorten the ion/electron path and improve the reaction homogeneity. Herein, this study reports a novel three-stage strategy (self-assembly of NiMn-LDH/ppy-C — reduction to NiMn/ppy-C — in situ phase transformation into NiMn/NiMn-LDH/ppy-C) to reduce the sheet size of NiMn-LDH to nanometer. Triggered by electrochemical activation, NiMn-LDH nanosheets can hereby easily and orderly grow on the exposed active (1 1 1) crystal plane of Ni to establish NiMn-LDH/NiMn heterostructure around ppy-C. Importantly, nanosizing and hierarchical structure play a synergistic role to maintain structural integrity and to promote the electron/mass transfer kinetics. The NiMn/NiMn-LDH/ppy-C composite delivers superior cycling stability with almost no decay of capacity retention after 40,000 cycles at 5 A g⁻¹. Our hierarchical morphology modulation provides an ingenious, efficient way to boost the performance of Ni-based layered hydroxide materials.