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Highlight • A two-step hydrothermal strategy is adopted to transform Ni 3 [Fe(CN) 6 ] 2 to NiFe 2 O 4. • NiFe 2 O 4 @rGO slice is prepared as electrode for flexible symmetric supercapacitor. • NiFe 2 O 4 @rGO electrode shows excellent specific capacitance and cycling stability. Abstract A high working voltage and specific capacitance are vital for flexible solid-state symmetric supercapacitor (FSSC) devices to achieve decent energy densities with high power. In this paper, we report a 1.8 V FSSC based on NiFe 2 O 4 nanocubes anchored on reduced graphene oxide (rGO) cryogel electrode. Through surface protection by a free-standing three-dimensional cross-linked network structure, NiFe 2 O 4 converted from Ni 3 [Fe(CN) 6 ] 2 inhibits the original nanocube structure. Benefiting from the synergistic effects between NiFe 2 O 4 nanocubes and graphene nanosheets, the newly synthesized NiFe 2 O 4 @rGO hybrid electrode delivers a high charge storage capacity (488 F g−1 at a constant current density of 1 A g−1), excellent rate ability and cycling performance (89.8% of the initial capacitance value after 10,000 cycles). In addition, NiFe 2 O 4 @rGO FSSC has been assembled and exhibits stable behavior at bend state, as well as high energy density of 62.5 Wh kg−1, and long cycle life (93.2% of the initial capacitance value after 6000 cycles). The proposed strategy for controlling the design and synthesis of NiFe 2 O 4 @rGO nanostructures provides promise for the development of high performance electrode in advanced energy storage devices. [ABSTRACT FROM AUTHOR]

The flexible solid-state supercapacitor (FSSC) has attracted many attentions due to its feature of high power density with stable cycling performance, as well as lightweight and flexible features and is expected as an ideal candidate power supply for portable and wearable electronics devices. In general, the electrode plays an important role in determining the overall performance of the FSSC. Therefore, to meet the requirement of practical applications, a simple, facile and environment friendly strategy to prepare deformable/flexible electrodes with high energy density is the target issue to be considered. Herein, we report a generalized “soaking-recrystallization-calcination” method to enhance the capacitance performance of commercialized carbon fiber cloth. Thanks to the in-situ etching process to increase the surface area and the synchronous heteroatom doping to induce pseudocapacitive behavior, the resultant activated carbon fiber cloth sample exhibits an ultra-high areal capacitance up to 362 mF cm −2 , is about 1448 fold enhancement than that of fresh carbon fiber cloth calcined at 750 °C. Meanwhile, the assembled FSSC based on the activated carbon fiber cloth exhibits a maximum volumetric energy density of 0.35 mWh cm −3 and gravimetric energy density of 0.84 Wh kg −1 . Such results represent a novel and promising direction to prepare high performance flexible electrode for FSSC application. [ABSTRACT FROM AUTHOR]

Flexible solid-state supercapacitor (FSSC) holds great promise as power source to supply the next generation of portable and wearable electronics. Assembling asymmetric supercapacitor constructed with broadening cell voltage ( V ) is the promising way to increase the energy density. However, the imparity reaction kinetics between EDLC and pseudocapacitive materials will further lead to inferior power density. Hence, to pursue higher working voltage and energy density, a hybrid configuration of cobalt hexacyanoferrate/reduced graphene oxide hydrogels (PB-Co/rGOH) is prepared through a one-pot hydrothermal method. With highly interconnected 3D network structure, excellent mechanical robustness and the synergistic effects between the graphene and PB-Co, the resultant PB-Co/rGOH exhibits a high specific capacitance of 220 F g −1 and well cycle stability (83% capacitance retention after 10,000 cycles at 5 A g −1 ). Moreover, the assembled PB-Co/rGOH//PB-Co/rGOH symmetric flexibly solid-state supercapacitor exhibits an amazing higher working voltage of 2.0 V and a remarkable energy density of 57.5 Wh kg −1 , which is comparable with that of Ni/MH batteries (60–120 Wh kg −1 ). These excellent electrochemical performances of the hybrid electrode provide a rational design strategy for developing supercapacitors with high energy density. [ABSTRACT FROM AUTHOR]

• Bimetallic (Ni,Mo)S 2 was synthesized through a two-step solvothermal approach. • The (Ni,Mo)S 2 /G composite exhibits high specific capacity of 951 C g−1. • The ASC device shows a ultrahigh energy density of 84.5 Wh kg−1. Thanks to their high electrical conductivity, electrochemical stability and activity, transition metal sulfides have been widely designed and developed for supercapacitors with excellent electrochemical performances. Herein, we report the NiS 2 /MoS 2 mixed phases with abundant exposed active edge sites decorated on graphene nanosheets (named as (Ni,Mo)S 2 /G) through a facile two-step hydrothermal approach. Benefitting from its unique chemical property and structure, the as-prepared (Ni,Mo)S 2 /G composite possesses impressive electrochemical performances as electrodes of battery-type supercapacitors in 2 M KOH, such as high specific capacity of 951 C g−1 (2379 F g−1) at 1 A g−1 with superb rate capability (60.7% at 100 A g−1). Additionally, the asymmetric supercapacitor (ASC) device assembled based on the active edge site-enriched (Ni,Mo)S 2 /G as positive electrode and nitrogen-doped porous graphene as negative electrode displays an ultrahigh energy density of 84.5 Wh kg−1, superior to those of the Ni- and Mo-based ASCs in aqueous electrolytes reported so far. Such novel strategy may hold great promise for exploring other polymetallic sulfides with abundant exposed active edge sites for energy storage and conversion. [ABSTRACT FROM AUTHOR]

• The PTC-S as anode has an outstanding performance in 0.5 M LiCl + 0.5 M MgCl 2 aqueous solution. • The PTC-S exhibits a good rate ability and cycling stability. • PTC-S‖LiMn 2 O 4 has a high capacity and excellent cycling stability. Aqueous batteries are appealing for large-scale storage applications, due to their high safety level, low cost, and excellent durability. In this study, we reported a new anode material, namely sulfur perylene-3,4,9,10-tetracarboxylate (PTC-S), which is more stable than other electrode materials used in aqueous Mg-Li ion batteries. When PTC-S is used as the anode in 0.5 M MgCl 2 + 0.5 M LiCl with a current density of 50 mA g−1, the discharge specific capacity is 287.3 mAh g−1 at the initial cycle and the capacity retention rate is still close to 100% at over 1000 cycles. The monomer structural material conjugated with bifunctional groups can provide the space for the intercalation of Mg2+ and Li+ at the same time, shorten the ion transmission path and accelerate the transmission speed of metal ions in the electrode. In order to develop aqueous battery as quickly as possible, LiMn 2 O 4 and PTC-S are used as cathode and anode materials, respectively, in a dual-ion salt aqueous battery. The PTC-S‖LiMn 2 O 4 battery exhibits a high capacity and an excellent cycling stability performance in aqueous Mg-Li ion battery. The battery has a high capacity performance of 240.0 mAh g−1 at a voltage ranging from 0.0 V to 1.8 V, as well as a high specific energy density of 172.8 Wh kg−1 and remarkable cycling stability. PTC-S in 0.5 M MgCl 2 electrolyte has a current density of 100 mA g−1, a specific discharge capacity of 203 mAh g−1 and a first-cycle Coulomb efficiency close to 100%. Under the same test conditions, the discharge specific capacity is higher than that of the perylene-3,4,9,10-tetracarboxylic dihydride (PTCI) electrode (101 mAh g−1), and the capacity retention rate is increased by 30.4%. [ABSTRACT FROM AUTHOR]

Flexible electrochemical energy storage devices have great potential in wearable and portable electronic devices. However, their practical applications have been deferred by mechanical damages such as repeated stretching, bending and squeezing. Self-healing hydrogel electrolytes can automatically repair such physical damages and maintain good electric contact at electrode/electrolyte interface. Herein, we report a hydrogel electrolyte with excellent tensile properties and good conductivity under large strain/stress. A solid state supercapacitor was further demonstrated, showing a high energy density of 21.3 Wh kg-1 at a power density of 350 W kg-1. The as-fabricated supercapacitor possesses good stretchability, with a 68% of retention of its initial capacitance after 40 breaking/healing cycles. The excellent self-healing capability of the hydrogel electrolyte can be attributed to the presence of hydrogen bonds and molecular chain fluidity within its structural motif. Our work provides promising routes towards developing new self-healing solid-state electrolytes for next-generation electrochemical energy storage and conversion applications with good performance and high safety. [ABSTRACT FROM AUTHOR]

• Ultrathin in-plane 1T-2H MoS 2 heterostructures are coaxially arrayed on 3D CFs. • The 1T-2H ultrathin heterostructures exhibit surprising structure stability. • Our ASC device exhibits an ultrahigh energy density of 81.4 Wh kg−1. Metallic 1T MoS 2 is a promising anode candidate for supercapacitors due to its intrinsically excellent electrical conductivity and high electrochemical activity. However, it is quite unstable and hard to be massively synthesized through common methods. Herein, structurally stable ultrathin (1–3 layers) in-plane 1T-2H MoS 2 heterostructures have been rationally modulated and coaxially aligned on three-dimensional carbon nanofibers (MoS 2 /CF) through a facile hydrothermal approach for supercapacitors and electrocatalysis. Benefiting from the unique heterostructure, the MoS 2 /CF composite shows amazing stability with no obvious change after being stored in air for over 36 months. In addition, it presents high specific capacitance of 310 F g−1 and remarkable rate capability of 78% at 100 mV s−1. The fabricated asymmetric supercapacitor delivers an impressive energy density of 81.4 Wh kg−‍‍‍‍‍1 in 1 M Na 2 SO 4 solution attributed to the high specific capacitance and large operating voltage range of 2 V. Moreover, the MoS 2 /CF composite also demonstrates enhanced electrocatalytic activity for hydrogen evolution reaction with a low overpotential of 194 mV at 10 mA cm−2. The work may promote the developments of high-performance bifunctional energy conversion and storage systems in future. [ABSTRACT FROM AUTHOR]

• A PPy-rGO Janus-faced film is prepared through a facile and scalable method. • The PPy-rGO electrode reveals a ultra-high specific capacitances of 1380 mF cm−2. • The assembled PPy-rGO//PPy-rGO device delivers a high energy density of 31.95 Wh L−1. The flexible supercapacitors have attracted tremendous attention, but challenges still remain in seeking suitable electrode materials to enhance the energy density and other aspects. To this end, a unique Polypyrrole (PPy)-reduced graphene oxide (rGO) Janus-faced film is prepared through a facile and scalable method consisting of the deposition of graphene film on the surface of copper foil via a Cu||GO electrochemical cell followed by the self-assembly of PPy at the heterogeneous interface. Such a distinctive structure, in which the PPy layer acts as the source of high pseudo-capacitance, while the graphene layer is employed as the "high way" for rapid electron transport and as well as the strong π-π coupling effect between graphene and polymer nanosheets, endows the resultant electrode ultra-high specific capacitances (1380 mF cm−2 at 1 mA cm−2) and excellent rate capability (65.1% capacitance retention with the current density increases to 20 mA cm−2). Furthermore, the assembled PPy-rGO//PPy-rGO symmetric supercapacitors deliver a maximum energy density of 31.95 Wh L−1, remarkable cyclic stability (89.7% capacitance retention after 10,000 cycles) and superior mechanical property (82% capacitance retention after 8000 cycles under different bending conditions). [ABSTRACT FROM AUTHOR]