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Novel supercapacitor electrodes comprising hierarchical architectures with high specific surface areas, unique porosities, excellent conductivities, and admirable mechanical stabilities are necessary for developing high-performance solid-state supercapacitors. Herein, a novel ultra-thin copper nickel sulfide (Cu1−xNixS) nanosheet array supercapacitor electrode was constructed on a 3D Ni backbone through a powerful anion exchange technique and it demonstrated a unique architecture with a substantial degree of porosity. Accordingly, Cu1−xNixS plays an imperative role in the electrochemical energy storage characteristics of the electrode by accomplishing an ultra-high areal capacitance of 5.88 F cm−2 and a specific capacitance of 2672 F g−1 at a current density of 2 mA cm−2 with an excellent rate capability (71.26% capacitance retention at 20 mA cm−2) and a superior cycling performance (97.33% capacitance retention after 10 000 cycles). To design asymmetric supercapacitors (ASCs), Cu1−xNixS and N, S co-doped graphene nanosheets (NSGNSs) are employed as positive and negative electrodes, respectively. Remarkably, the fabricated ASC exhibits a potential window of ∼1.8 V, which demonstrates an ultra-high energy density of ∼94.05 W h kg−1 at 1.09 kW kg−1 as well as an excellent life cycle (95.86% capacitance retention after 10 000 cycles). Owing to this fact, this investigation offers a simple, scalable, and cost-effective approach for the fabrication of other ternary transition metal sulfides (TMSs), emphasizing great prospects in next-generation energy storage applications.

A unique morphology, high specific surface area, extraordinary porosity, and excellent conductive networks are typical favorable properties of pseudocapacitors; however, fully comprehending and interpreting this substantive topic still remains a great challenge. Herein, we present a new strategy for the direct growth of a cobalt monoxide@manganese oxide core–shell nanostructure on 3D Ni foam (CoO@MnO2/Ni foam). This is accomplished by simple, scalable, in situ fabrication methods to produce a material that can be employed as an advanced electrode material for high-energy solid state asymmetric supercapacitors (ASCs). The cost-effective, binder-free 3D CoO@MnO2 core–shell nanostructure delivers excellent electrochemical properties with an ultra-high specific capacitance (1835 F g−1 at a current density of 1 A g−1), tremendous rate capabilities with an extraordinary capacitance of 1198 F g−1 at a current density of 20 A g−1, and outstanding stability (97.7% capacitance retention after 10 000 cycles). ASCs with a maximum potential window of 1.8 V are fabricated by using a 3D CoO@MnO2 core–shell nanohybrid as the positive electrode and N-doped graphene (NG) as the negative electrode in order to validate the outstanding performance for practical energy storage devices. Impressively, the ASCs delivered a high specific capacitance (191 F g−1 at 1 A g−1), excellent energy density (∼85.9 W h kg−1), an ultra-high power density (∼16 769 W kg−1 at 51.7 W h kg−1), and remarkable cycle stability (86.8% capacitance retention after 10 000 cycles). These findings provide a new method to design 3D CoO@MnO2 core–shell nanostructures that are cost-effective and binder-free electrode materials for the development of high-performance energy storage devices.

A novel strategy for the synthesis of high-quality ternary cobalt copper sulfide nanoparticles (NPs) anchored on nitrogen doped graphene nanosheets (Co2CuS4/NG) was developed via a one-pot solvothermal method. FE-SEM and TEM images showed that the Co2CuS4 NPs with an average size of ∼21 nm were anchored to NG nanosheets. The NG nanosheets provide a large surface area to reduce self-aggregation and confine the shape of the Co2CuS4 NPs for a highly conductive network to boost the charge transport properties of energy storage devices. Impressively, the synergetic Co2CuS4/NG composite showed a high specific capacitance of ∼1005 F g−1 at 1 A g−1, excellent rate capability (770 F g−1 at 50 A g−1), and outstanding stability (96.3% capacitance retention after 5000 cycles). The electrochemical performance of the Co2CuS4/NG composite was superior to that of monometallic CoS/NG, Cu2S/NG composite, pure Co2CuS4, and NG. An asymmetric supercapacitor device fabricated using the Co2CuS4/NG composite as the positive electrode material and NG as the negative electrode material illustrates the outstanding performance for practical energy storage devices. The asymmetric supercapacitor device delivers superb energy density (53.3 W h kg−1), high power density (∼10 936 W kg−1 at 38.4 W h kg−1), and a long-cycle life (∼4000 times).

A novel three-dimensional (3D) hierarchical hybrid architecture, consisting of in situ designed cobalt-encapsulated nitrogen doped carbon nanotubes (Co–NCNTs) grown on nitrogen doped graphene (NG), is fabricated for asymmetric supercapacitors. When evaluated as an electrode material for supercapacitors, the 3D hybrid has an excellent energy density, outstanding rate capability and long-cycle life compared with commercial electrode materials. The decent electrochemical performance is comparable to most of the earlier reported results and the synergistic effect boosts the pseudocapacitive performance. The constructed hybrid exhibits excellent energy storage characteristics, which result in an ultra-high specific capacitance of 2568 F g−1 at 2 A g−1 and excellent rate capability with an extraordinary capacitance of 1594 F g−1 at 100 A g−1 (96.64% capacitance retention after 20000 cycles). The improvement in the outstanding electrochemical performance can be attributed to the unique morphology, extraordinary porosity, excellent conductive networks, and the intense networking of Co–NCNT and NG nanosheets in the 3D hybrid. An asymmetric supercapacitor fabricated using the 3D NG/Co–NCNT hybrid as the positive electrode and NG as the negative electrode demonstrates exceptional performance for practical energy storage devices. The assembled asymmetric supercapacitors provide a greater energy density (∼88.44 W h kg−1), an ultra-high power density (∼17991 W kg−1 at 56.97 W h kg−1), and outstanding cyclability (∼10000 times).