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In this article, ZnCo 2 O 4 nanowires deposited with two kinds of typical layered double hydroxides (Ni–Al,Co–Al LDH) are developed via scalable method. Two materials all display core–shell hierarchical structure. High specific capacitance of 2041 F g−1 and 1586 F g−1 are obtained for ZnCo 2 O 4 @Co–Al LDH and ZnCo 2 O 4 @Ni–Al LDH,respectively. Combining with active surface and synergistic effect, the role of hierarchical structure in enhancing performance is revealed. Moreover, two all solid state supercapacitors based on fabricated materials as positive electrodes, activated carbon as negative electrodes and PVA–KOH as polymer electrolyte are assembled. The maximum power and energy densities of ZnCo 2 O 4 @Co–Al LDH//AC are 6200 W kg−1 and 50.1 Wh kg−1, respectively. While the power and energy densities of ZnCo 2 O 4 @Ni–Al LDH//AC are 3400 W kg−1 and 27.8 Wh kg−1. At last, an energy storage–conversion system, based on solar cell as input device and assembled asymmetric supercapacitor ZnCo 2 O 4 @Co–Al LDH//AC as output device, is integrated as a self–sustaining power device, indicating its potential in practical applications. In this article, ZnCo 2 O 4 nanowires deposited with two kinds of typical layered double hydroxides (LDHs) are developed via scalable method. Combining with active surface and synergistic effect, the role of hierarchical structure of each material in enhancing performance is revealed. Moreover, an energy storage–conversion system, based on solar cell as input device and assembled asymmetric supercapacitor as output device, is integrated as a self–sustaining power device, further indicating its potential in practical applications. Image 1 [ABSTRACT FROM AUTHOR]

Highlights: A freestanding MXene-derived defect-rich TiO2@reduced graphene oxides (M-TiO2@rGO) foam electrode was fabricated. M-TiO2@rGO presents fast Na+ storage kinetics due to capacitive contribution. M-TiO2@rGO foam electrode displays a capacity retention of 90.7% after 5000 cycles. Sodium ion batteries and capacitors have demonstrated their potential applications for next-generation low-cost energy storage devices. These devices's rate ability is determined by the fast sodium ion storage behavior in electrode materials. Herein, a defective TiO2@reduced graphene oxide (M-TiO2@rGO) self-supporting foam electrode is constructed via a facile MXene decomposition and graphene oxide self-assembling process. The employment of the MXene parent phase exhibits distinctive advantages, enabling defect engineering, nanoengineering, and fluorine-doped metal oxides. As a result, the M-TiO2@rGO electrode shows a pseudocapacitance-dominated hybrid sodium storage mechanism. The pseudocapacitance-dominated process leads to high capacity, remarkable rate ability, and superior cycling performance. Significantly, an M-TiO2@rGO//Na3V2(PO4)3 sodium full cell and an M-TiO2@rGO//HPAC sodium ion capacitor are fabricated to demonstrate the promising application of M-TiO2@rGO. The sodium ion battery presents a capacity of 177.1 mAh g−1 at 500 mA g−1 and capacity retention of 74% after 200 cycles. The sodium ion capacitor delivers a maximum energy density of 101.2 Wh kg−1 and a maximum power density of 10,103.7 W kg−1. At 1.0 A g−1, it displays an energy retention of 84.7% after 10,000 cycles. [ABSTRACT FROM AUTHOR]

Abstract: Ni(OH)2 nanosheets are directly grown on nickel foam by a simple template-free growth process. Their microstructure and surface morphology are studied by X-ray diffraction spectroscopy and scanning electron microscopy. The XRD and SEM results show that Ni(OH)2 has a β-phase structure and covers the nickel foam skeleton with nanosheets. This β-Ni(OH)2/Ni-foam electrode exhibits a high specific electric quantity of 790.3 C g−1 approaching the theoretical value (1040.6 C g−1) and high electrochemical activity. Asymmetric supercapacitor has been fabricated successfully using β-Ni(OH)2/Ni-foam nanosheets as positive electrode and activated carbon as negative electrode in a KOH aqueous electrolyte. The electrochemical capacitances of this supercapacitor are investigated by cyclic voltammetry, galvanostatic charge/discharge and electrochemical impedance spectroscopy. An asymmetric supercapacitor AC/6 mol L−1 KOH/β-Ni(OH)2/Ni-foam could be cycled reversibly in the high-voltage region of 0–1.6 V and displays intriguing performances with a specific capacitance of 105.8 F g−1 and high energy density of 36.2 W h kg−1. Importantly, this asymmetric supercapacitor device exhibits an excellent long cycle life along with 92% specific capacitance retained after 1000 cycles. [Copyright &y& Elsevier]

Binary metal niobium oxides can offer a higher specific capacity compared to niobium pentoxide (Nb 2 O 5) and thus are ideal anode candidates for lithium ion capacitors (LICs). However, their lower electronic conductivity limits their ability to achieve high energy and power densities. In this paper, one-dimensional (1D) copper niobate (CuNb 2 O 6) nanowires are successfully prepared by electrospinning technology and then immobilized on two-dimensional (2D) reduced graphene oxide (rGO) nanosheets to form a unique 1D nanowire/2D nanosheet CuNb 2 O 6 /rGO structure. The 1D/2D CuNb 2 O 6 /rGO electrode exhibits a high specific capacity of 312.2 mAh g−1 at 100 mA g−1 as the anode of LICs. The proposed Li+ storage mechanism of the CuNb 2 O 6 anode involves CuNb 2 O 6 decomposition into lithium niobate (Li 3 NbO 4) and copper (Cu) during the initial lithium insertion process. The intercalation-type Li 3 NbO 4 will further serve as the host to Li+ and the inactive Cu phase will act as a conductive network for electron transportation. Furthermore, the energy density of the assembled CuNb 2 O 6 /rGO//activated carbon (CuNb 2 O 6 /rGO//AC) device could achieve a value as high as 92.1 Wh kg−1 and could thus be considered as a possible alternative electrode material for high energy and power LICs. [ABSTRACT FROM AUTHOR]

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]

Graphical abstract Abstract Unique nanostructure, high electrical conductivity, satisfactory energy density, and extraordinary cycling stability are important evaluation criteria for high-efficient energy storage devices. Herein, Fe 3 O 4 nanospheres are successfully in situ decorated on graphene nanosheets through an environmentally benign and facile solvothermal procedure. When utilized as an electrode for supercapacitor, the graphene/Fe 3 O 4 nanocomposite exhibits a notably enhanced specific capacity (268 F·g−1 at 2 mV·s−1) and remarkable cycling performance with 98.9% capacity retention after 10,000 cycles. Furthermore, the fabricated graphene/MnO 2 //graphene/Fe 3 O 4 asymmetric supercapacitor device displays a desirable energy density (87.6 Wh·kg−1) and superior cycling stability (93.1% capacity retention after 10,000 cycles). [ABSTRACT FROM AUTHOR]

Graphical abstract Abstract Flexible supercapacitor plays a progressively more important part in power source for smart electronic devices and how to enhance its energy density is the urgent issue to be addressed. Hence, a hybrid electrode of Polypyrrole@reduced graphene oxide hydrogel (PPy@rGOH) is synthesized via a combine hydrothermal treatment of GO solution to assemble hydrogel and subsequently in-situ electropolymerization preparation of PPy on the surface of graphene. Through controlling the time of electropolymerization, the resultant PPy@rGOH-20 s with high specific surface area exhibits an excellent specific capacitance of 340 F g−1 at a current density of 1 A g−1 and superior cycling stability of 87.4% capacitance retention after 10,000 charging/discharging cycles at 3 A g−1 in 1 M KNO 3. The assembled flexible asymmetric supercapacitor (FASC) by employing the PPy@rGOH-20s as positive electrode and pure rGOH as negative electrode presents a maximum operational voltage window of 1.6 V and high energy density of 46.9 W h kg−1, which is higher than polymer/carbon-based supercapacitors previously reported. [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]

• α-MnSe Nanosheets are prepared via a facile hydrothermal method. • The effect of reaction time on electrochemical performance is investigated. • The α-MnSe electrode delivers a high capacity of 88.3 mAh g−1 at 1 A g−1. • The asymmetric supercapacitor exhibits a high energy density of 39.3 Wh kg−1. Transition metal selenides are regarded as emerging materials for energy storage devices because of their good electrical conductivity and electrochemical activity. Here, a binder-free ultrathin α-MnSe nanosheets electrode is prepared and the supercapacitor performance is comprehensively explored. Due to the increased active sites, enlarged contact area for electrolyte, as well as shorten ions diffusion pathway, the prepared electrode delivers high capacity of 88.3 mAh g−1 at 1 A g−1, good rate capability, and long-term durability (91% remain after 5000 cycles). Moreover, the asymmetric supercapacitor, fabricated by α-MnSe anode and active carbon cathode, displays a high energy density of 39.3 Wh kg−1 at a power density of 0.92 kW kg−1 and satisfying cycle performance. This study demonstrates that the binder-free α-MnSe electrode holds great promise for supercapacitor. [ABSTRACT FROM AUTHOR]

Developing novel materials with rational structures and excellent electrical conductivity is vitally important for energy storage devices. Herein, hollow cobalt molybdenum selenide (Co–Mo–Se) nanosheet arrays are fabricated via a self-sacrificing template method and selenization process, where cobalt-organic framework serves as the template. Benefiting from unique hollow nanoarrays structure, the Co–Mo–Se electrode offers rich electroactive sites, large accessible regions for electrolyte, and short ions diffusion pathways. Additionally, it is observed that the Co–Mo–Se possesses a low charge transfer resistance owing to the intrinsic metallicity. As a result, the Co–Mo–Se electrode exhibits favorable energy storage properties, including high capacity (221.7 mAh g−1), good rate property, and outstanding stability (95% after 8000 cycles). More importantly, the assembled Co–Mo–Se//active carbon (AC) achieves high energy density (44.7 Wh kg−1) and remarkable durability. Notably, two hybrid devices connected in series successfully power an electronic watch for 70 min, demonstrating its practical applicability. These results indicate that the synthesized hollow Co–Mo–Se nanosheet arrays have promising applications as electrode materials for high-performance energy storage devices. • Co-MOF was employed as template to obtain hollow Co–Mo–Se nanosheet arrays. • The Co–Mo–Se delivers a specific capacity of 221.7 mAh g−1 at 1 A g−1. • The ion exchange/etching method was applied in this work. • The asymmetric supercapacitor delivers high energy and power densities. [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]

NiS 2 is a promising anode material for sodium-ion batteries (SIBs) and capacitors (SICs). However, the sluggish Na+ diffusion and large volume change of bulk NiS 2 during sodiation/de-sodiation lead to poor rate capability and fast capacity decay, limiting its practical application. Herein, we design and prepare well-oriented NiS 2 nanosheets on porous carbon microtubes (denoted as NiS 2 /pCMT) as a novel anode material for SIBs/SHCs. The unique porous hollow carbon tubes and NiS 2 nanosheets can well relieve the repeated stress/strain and maintain the structural integrity of the composite anode during long-term charging/discharging. As a confirmation, a modelled SHC is constructed by using the NiS 2 /pCMT composite as anode and coupling with an activated carbon cathode, delivering a high energy density of 136 Wh kg−1 and good cycling stability. The first-principles density functional theory (DFT) calculations confirm that the NiS 2 nanosheets surface has a high chemical affinity towards Na+ ions, promising the concentration of Na+ ion on/nearby the surface for fast redox reactions during sodiation/de-sodiation of NiS 2. This work provides some new insights for the design and fabrication novel composite electrode materials for applications in beyond lithium-ion batteries/capacitors. • The carbon microtubes have unique tubular structure and good conductivity. • NiS 2 nanosheets uniformly grow on both sides of the carbon microtubes. • The layered NiS 2 nanosheets facilitate the intercalation of the Na+ ions. • The sodium-ion hybrid capacitor delivers high energy and power densities. [ABSTRACT FROM AUTHOR]