Hierarchical NiO mesocrystals with tuneable high-energy facets for pseudocapacitive charge storage

Mesocrystals are advantageous in providing a large specific surface and favorable transport properties, and have been extensively studied for energy-related applications including supercapacitors, solar cells, lithium-ion batteries, and catalysis. However, the practical applications of mesocrystals are hindered by many obstacles, such as high cost, complicated synthesis processes, and utilization of deleterious additives. Herein, we report a facile one-step and additive-free route for the controllable synthesis of NiO mesocrystals (NOMs) with a cuboctahedral morphology and layered hierarchical structures consisting of self-assembled NiO nanosheets. When employed as an electrode material for supercapacitors, the as-prepared NOMs exhibited an exceptional electrochemical performance such as an ultrahigh reversible specific capacity of ca. 1039 F g−1 at a current density of 1.0 A g−1 and excellent cycling stability (ca. 93% capacitance retention after 10 000 charge/discharge cycles). Moreover, an all-solid-state hybrid supercapacitor based on hierarchical NOMs and three-dimensional nitrogen-doped graphene manifested a high energy density of 34.4 W h kg−1 at a power density of 150 W kg−1 in 2.0 M KOH aqueous electrolyte. These results further demonstrate the potential of NiO mesocrystals as a promising electrode material by constructing a hierarchical mesostructure, which can improve the electrochemical performance for energy storage. The outstanding electrochemical performance may be attributed to their hierarchical mesostructure that can effectively enhance the electrical conductivity and avoid the aggregation of NiO nanosheets, and the exposed {100} facets with a high electrochemical activity. © The Royal Society of Chemistry.