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DFT calculation is used to study the electrochemical capacity enhancement mechanism of the fabricated flexible 3D porous rOHNM-AGs electrodes based on open-hollow Ni-MOF microspheres with high mechanical strength and superior electrochemical properties. [Display omitted] • 3D rOHNM-AGs are achieved by embedding open-hollow Ni-MOF microspheres into graphene nanosheets. • DFT calculation reveals charge-transfer interaction between the rOHNM-AGs and OH– ions. • The rOHNM-AGs/KOH/PVA film can be twisted with different angles, which can lift 500 g plastic bottle. • The fabricated rOHNM-AGs electrode exhibit superb specific capacitance of 1644F·g−1 at 1 A·g−1. • A portable multifunctional instrument can be powered by all-solid-state supercapacitor device for 15 mins. Metal-organic frameworks (MOFs) are extensively used for electrode materials of supercapacitors under their unique characteristics like customizable pore size, plentiful active sites and tunable structure. However, the MOFs lack adequate electrical conductivity and satisfactory stability, when directly applied to supercapacitor electrode materials, limiting the further improvement of their electrochemical properties. Accordingly, three-dimensional porous aerogels (rOHNM-AGs) have been achieved by embedding open-hollow nickel-based metal–organic framework microspheres between graphene layers. Under the controllable and highly ordered metal nodes as well as organic linkers, the prepared rOHNM-AGs still reserve the preponderance of MOF materials with multifarious exceptional constituent and configurational benefits. Furthermore, the remarkable electrical conductivity from graphene leads to a significant increase in electron/ion transport rate. In addition, charge-transfer interaction between the acceptor of OH– ions and the donor of rOHNM-AGs has been exposed by the density functional theory calculations. Moreover, a pliable and high tensile rOHNM-AGs/PVA/KOH film electrode has been fabricated by the PVA/KOH gel-electrolyte, which is capable of curving at multifarious angles. For actual utilizations, the manufactured supercapacitor apparatus can run a multi-purpose display for over 15 mins. Therefore, this groundbreaking research furnishes a new inspiration for preparing composite electrodes based on MOFs and graphene for flexible asymmetric supercapacitors. [ABSTRACT FROM AUTHOR]

[Display omitted] Ortho-hexagonal and highly-oriented NiMnCo-LDH/ZnO@CC self-supporting electrode derived from ZIF-67 covered ZnO nanorod-arrays is fabricated and employed for portable asymmetric solid-state supercapacitor. • Novel ortho -hexagonal NiMnCo-LDH has been synthesized. • ZIF-67 covered ZnO nanorod-arrays as self-supporting electrode is synthesized. • The fabricated electrodes exhibit superior electrochemical properties. • A multifunctional instrument can be powered for more than 30 mins. • The device can be carried outdoors to monitor time, temperature and air humidity. Metal-organic frameworks have attracted much attention due to their abundant redox sites and tunable characteristics, which are advantageous for energy storage applications. However, the low electrical conductivity, poor physical strength and undesirable capacity seriously hinder their applications. Therefore, designing effective and convenient strategies to build composites with unique structures will be of practical significance. Herein, we successfully generate NMC-LDH/ZnO@CC nanocomposites by growing ortho -hexagonal nickel–cobalt layered double hydroxide (NMC-LDH) nanosheets in-situ on ZIF-67 precursor covering vertical arrays of ZnO nanorods. As a result of the unqiue ortho -hexagonal structure, highly ordered arrangement of active substances and multi-dimensional spaces of the prepared NMC-LDH/ZnO@CC binder-free electrode, its capacitance is as high as 9258 mF cm−2 at a current density of 2 mA cm−2 and the capacitance retention is maintained at 87.5 % after 5000 cycles. Furthermore, in order to explore the practical value of the prepared binder-free electrode, the NMC-LDH/ZnO@CC//AC solid-state asymmetric supercapacitor device is assembled. The energy density of the assembled supercapacitor is 24.6 W h kg−1 at a power density of 170 W kg−1 and 1020 W kg−1 at an energy density of 11.8 W h kg−1. In addition, a versatile instrument for monitoring air humidity, time and ambient temperature in portable environments can be powered by a single ultracapacitor unit for more than 30 min. Overall, this study provides a unique strategy for synthesizing ZIF derivatives with novel morphologies for electrochemical energy storage applications. [ABSTRACT FROM AUTHOR]