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An efficient approach to increase the energy density of supercapacitors is to prepare electrode materials with larger specific capacitance and increase the potential difference between the positive and negative electrodes in the device. Herein, an organic molecular electrode (OME) is prepared by anchoring 1,10‐phenanthroline‐5,6‐dione (PD), which possesses two pyridine rings and an electron‐deficient conjugated system, onto reduced graphene oxide (rGO). Because of the electron‐deficient conjugated structure of PD molecule, PD/rGOs exhibit a more positive redox peak potential along with the advantages of high capacitance‐controlled behaviour and fast reaction kinetics. Additionally, the small energy gap between the lowest unoccupied molecular orbital (LUMO) and highest occupied molecular orbital (HOMO) leads to increased conductivity in PD/rGO. To assemble the asymmetric supercapacitor (ASC), a two‐dimensional metal carbide, as known as MXene, with a chemical composition of Ti3C2Tx is selected as the negative electrode due to its exceptional performance, and PD/rGO‐0.5 is employed as the positive electrode. Consequently, the working voltage is expanded up to 1.8 V. Through further electrochemical measurements, the assembled ASC (PD/rGO‐0.5//Ti3C2Tx) achieves a remarkable energy density of 36.8 Wh kg−1. Remarkably, connecting two ASCs in series can power 73 LEDs, showcasing its promising potential for energy storage applications. [ABSTRACT FROM AUTHOR]

A new redox‐active organic molecule, naphthalene diimide derivative (NDI), is synthesized through the condensation reaction for electrochemical energy storage, in which 1,4,5,8‐naphthalenetetracarboxylic dianhydride and 4‐aminophenol are used as skeleton and substituent, respectively. The NDI is acted as a guest molecule to non‐covalently modify reduced graphene oxide (rGO) and to form an organic molecular electrode (OMEs). The resultant electrode exhibits outstanding performance under the three‐electrode configuration, including specific capacitance (354 F g−1 at 5 mV s−1) and cycling performance (87.2% after 8000 cycles). Furthermore, the electrochemical behaviors of the OMEs are mainly controlled by surface reactions and pseudocapacitance contribution is up to 93% of the total capacity at 100 mV s−1. In addition, a positive electrode (graphene hydrogel‐2,6‐dihydroxynaphthalene (GH‐DN)) is formed by hydrothermal method. At last, an asymmetric device (GH‐DN//rGO‐NDI, ASC) is assembled and a specific capacitance of 111.3 F g−1 is reached. The ASC can deliver a high energy density of 26.3 Wh kg−1 at power density of 0.6 kW kg−1. Moreover, two ASC devices in series may light 81 light‐emitting diodes. It is believed that organic molecule electrodes are candidates for new green energy storage materials. [ABSTRACT FROM AUTHOR]

The design and preparation of electrode materials with unique nanostructure are regarded as a significant strategy to increase the capacitance and cycling stability of energy storage devices. Herein, a starfish-like core–shell Ni(OH)2@CoS material grown on Ni foam (Ni(OH)2@CoS/NF, denoted as NOCS-1/NF) was successfully fabricated via a stepwise hydrothermal method. Benefiting from the unique starfish-like core–shell nanostructure, obvious and abundant heterogeneous interfaces, and good synergy between every component, the specific capacitance of the as-prepared Ni(OH)2@CoS-1/NF electrode can reach up to 981 F g−1 at 1 A g−1 and maintained 73.2% of initial value at a high current density of 10 A g−1 in 2 M KOH aqueous solution. Moreover, a hybrid supercapacitor was prepared by using core–shell NOCS-1/NF as positive electrode and activated carbon coated on the NF (AC/NF) as negative electrode. The HSC delivered a high energy density of 17.9 Wh kg−1 at a power density of 749 W kg−1 and a satisfying cycling life with 90.1% capacitance retention after 4000 cycles. Eventually, two such devices in series successfully illuminated a red light-emitting diode. Meanwhile, this work probably provides a simple and convenient strategy to fabricate novel materials for the applicability of various energy-related fields. [ABSTRACT FROM AUTHOR]

2,6-Diaminoanthraquinone (DQ) molecules were covalently modified onto the surface of graphene (GO) via a nucleophilic displacement reaction between the epoxy groups on the surface of GO and the –NH2 groups of DQ molecules in the presence of ammonia to form a composite material (labeled as DQ–RGO). The rapid reversible faradaic reactions of DQ molecules are realized by means of the good conductivity of graphene. Therefore, the DQ–RGO composite material can combine the Faraday pseudocapacitance of DQ with the double-layer capacitance of graphene, thus displaying outstanding electrochemical performance in acidic electrolyte solution, including a high specific capacitance (332 F g−1 at 1 A g−1), excellent rate capability (the capacitance retention rate is 72.9% at 50 A g−1) and good cycling stability (maintaining 81.8% of the initial capacitance after 5000 cycles). Meanwhile, a thionine-functionalized graphene hydrogel (Th–GH) was also prepared via a non-covalent strategy. Finally, the DQ–RGO composite acted as the negative electrode and Th–GH acted as the positive electrode to construct an asymmetric supercapacitor (ASC). The ASC exhibited an energy density of 14.2 W h kg−1 along with a power density of 0.763 kW kg−1 and long cycling durability (maintaining 80% of the initial capacitance after 8000 cycles at 5 A g−1). More importantly, two such devices in series successfully illuminated 16 red light-emitting diodes (LEDs), demonstrating its outstanding energy storage performance. This work can provide ideas for the construction of green, all-carbon and excellent electrochemical performance devices. [ABSTRACT FROM AUTHOR]

[Display omitted] • A new electrode material (CHY/RGO) is prepared. • Chrysin (CHY) are grafted onto the surface of Reduced graphene oxide (RGO) by π-π electrostatic force. • The specific capacitance of CHY/RGO can reach up to 707F g−1 at 1 A g−1. • Density functional theory (DFT) calculation shows CHY are parallel adsorbed on RGO. • CHY/RGO//CHY/RGO device can deliver the energy density of 38 Wh kg−1. In this study, chrysin (CHY) molecules are immobilized on the surfaces of graphene oxide (GO) via π-π interactions to obtain organic molecular-modified reduced graphene oxide (RGO) composite electrode material (CHY/RGO) by one-step hydrothermal. On one hand, CHY molecules can contribute to capacitance through faradic reactions. On the other hand, they act as spacers that impede the accumulation of graphene nanosheets and promote electrolyte ion migration. As a result, CHY/RGO exhibits excellent capacitance performance. The specific capacitance is up to 707F g−1 (1 A g−1), and the capacitance remains 100% after 10 000 circles. In addition, the symmetrical supercapacitor (CHY/RGO//CHY/RGO) displays excellent energy storage performance, achieving an energy density of 38 Wh kg−1 at a power density of 800 W kg−1. Two CHY/RGO//CHY/RGO devices in series is capable of lighting 50 LEDs. Density functional theory (DFT) calculations show that CHY molecules are adsorbed parallel to the RGO by the π-π stacking. The DFT calculations also indicate that the modification of CHY molecules alters the charge distribution on the surface of RGO. Therefore, CHY/RGO composites offer a higher capacitance and superior cycle stability, making them a promising choice for future energy storage electrode materials. [ABSTRACT FROM AUTHOR]

Graphene hydrogels (GH), as a derivative of graphene have become a research hotspot in the field of energy storage due to their three-dimensional network structure which can prevent the agglomeration of graphene. The specific capacitance and energy storage ability can be further increased by non-covalent functional graphene hydrogels with organic small molecules. In this work, 4-methylumbelliferone (DTBF) molecules interacted on the surfaces of GH via π-π interactions to get a carbon electrode material (DTBF/GH) by one-step hydrothermal. On the one hand, the DTBF molecules can contribute capacitance by faradic reactions, on the other hand, they can act as spacers to hinder the accumulation of graphene nanosheets, thus enhancing the specific surface area of graphene and promoting the migration of electrolyte ions. As a result, DTBF/GH displays an ultrahigh-specific capacitance. The specific capacitance can reach up to 578 F g−1 (1 A g−1). To verify the influence of electrode material matching on capacitor performance, an asymmetric supercapacitor and a symmetrical capacitor are assembled respectively. Although the specific capacitance of the DTBF/GH material is higher than that of activated carbon (AC), the energy density (E d = 19 Wh kg−1) of the DTBF/GH//AC capacitors is higher than that of the DTBF/GH//DTBF/GH capacitors. It shows that the matching of electrode materials has a great influence on the E d and the power density (P d) of the capacitor. In addition, two DTBF/GH//AC devices in series can light 47 LEDs. [Display omitted] • A new carbon electrode material (DTBF/GH) is prepared. • GH with 3D network structure is conducive to the migration of electrolyte ions. • The specific capacitance of DTBF/GH can reach up to 578 g−1 at 1 A g−1. • The DTBF/GH //AC displays energy density of the 19 Wh kg−1. [ABSTRACT FROM AUTHOR]

Rational design and construct heterointerfaces of noble-metal-free materals is of very important to prepare high-performance electrocatalysts for hydrogen evolution reactions (HER). Herein, a novel 3D core-shell NiS@CoS@CC with abundant heterointerfaces is synthesized via a three-step strategy. The three-steps involve the rectangular Co(OH) 2 nanosheet arrays were grown on the CC, Ni(OH) 2 nanowires further grown on the Co(OH) 2 nanosheets to form a novel core-shell architecture (that is, nanosheets wrapped with nanowires), and the conversion of hydroxides to sulfides. In the 3D NiS@CoS@CC heterostructure, NiS are dispersively distributed on the surface of rectangular CoS nanosheets to form abundant heterointerface active sites, meanwhile, a large number of tiny pores are uniformly distributed over the core-shell structure due to the conversion of hydroxides to sulfides. The abundant NiS@CoS core-shell heterointerfaces can decrease the free energy of adsorption of H ads and enhance electronic conductivity through electronic coupling effects between different components, facilitate the electron transfer from the CoS nanosheets to the surrounding NiS. Furthermore, 3D porous structure can provide abundant edge sites and more electroactive surface area, and can accelerate the diffusion of gaseous products. Consequently, the as-prepared NiS@CoS@CC electrocatalyst presents remarkably enhanced performance for the HER in alkaline medium. The overpotential for HER is as low as 30 mV at a current density of 10 mA cm−2. Correspondingly, the Tafel slope of the electrode reaction is 97 mV dec−1. Particularly, the catalyst maintained a high stability (the final polarization curves suffer negligible degradation in comparison with the initial after taking 1000 continuous CV). The work provides a viable technical solution for fabricating heterostructure materials with excellent performances for future energy storage and conversion devices. Image 1 • NiS@CoS@CC catalysts with abundant heterointerfaces are designed and prepared. • Large number of pores are uniformly distributed over the NiS@CoS@CC catalyst. • The precursor is a novel core-shell architecture (nanosheets wrapped with nanowires). • NiS@CoS@CC presents excellent performance for the HER. [ABSTRACT FROM AUTHOR]

Design and fabrication of electrochemical energy storage systems with both high energy and power densities are of great importance. The battery-supercapacitor hybrid device (BSH), as one of these systems, has attracted enormous attentions. In this study, a battery-supercapacitor hybrid device was successfully fabricated by using the resultant 3D branched nanoarchitectures carbon nanotubes/Ni(OH) 2 (CNTs/Ni(OH) 2 ) as a positive electrode and the hierarchically porous, nitrogen-doped, interconnected carbon nanosheets (HPN-CNS) as the negative electrodes, respectively. HPN-CNS were prepared from agaric through simultaneous carbonization, activation, and nitrogen-doping method, while 3D branched nanoarchitectures CNTs/Ni(OH) 2 were prepared by deposited Ni(OH) 2 nanosheets on the highly conductive CNTs by a single-step chemical bath deposition. Because of their unique structure, both of the two materials exhibited excellent electrochemical performance. The as-assembled BSH delivered a high energy density of 34 W h kg -1 along with power density of 0.8 kW kg −1 , even at the power density of 16 kW kg −1 , energy density still hold at 22.2 W h kg -1 with the high potential window of 1.6 V. Furthermore, the device showed a good cycling stability with capacitance retention of 75% after 2000 cycles. Such results showed that HPN-CNS and CNTs/Ni(OH) 2 could be expected to serve as promising candidates for assembling high-performance BSH devices. [ABSTRACT FROM AUTHOR]

Further increasing the energy density of supercapacitors without reducing their high power density and stability remains a challenge. Organic quinone molecules have demonstrated potential in electrochemical energy storage on account of their excellent electrochemical activity and reversibility. Herein, 2-amino-3-chloro-1,4-naphthoquinone (2-NTQ) is covalently connected to the reduced graphene oxide (RGO) to obtain a new all‑carbon electrode material (2-NTQ-RGO). The 2-NTQ-RGO composite exhibits excellent capacitance performance by incorporating the merits of the 2-NTQ molecules and RGO. The optimized 2-NTQ-RGO possesses a high specific capacitance of 453 F g−1 at 1 A g−1 and displays good cycle stability (83% of the initial after 8000 cycles) in 1 M H 2 SO 4 electrolyte. Moreover, two asymmetric supercapacitors are assembled for the purpose of investigating the influence of the electrode materials matching on the performance of the capacitor. With the same positive material, the 2-NTQ-RGO//DQ-RGO can achieve an energy density of 23.4 Wh kg−1 and a power density of 900 W kg−1. Two ASC devices in series can light up in the shape of a "butterfly" consisting of 71 light-emitting diodes (LEDs). In contrast, the energy density of the 2-NTQ-RGO//AC is only 16.7 Wh kg−1 (812 W kg−1). The covalent grafting offers a new promising and effective method for the preparation of green all‑carbon energy storage materials. [Display omitted] • A new all‑carbon electrode material (2-NTQ-RGO) is prepared. • 2-NTQ is covatently grafted onto the surface of RGO. • The specific capacitance of 2-NTQ-RGO can reach up to 453 g−1 at 1 A g−1. • For comparison, two asymmetric supercapacitors are constructed. • The 2-NTQ-RGO//DQ-RGO displays a high energy density of the 23.4 Wh kg−1. [ABSTRACT FROM AUTHOR]

Transition metal sulfides (TMSs) have been widely researched as promising electrode materials for supercapacitors because of their high theoretical capacitance and rich redox reactive sites. In this work, tremella-like core-shell Co 9 S 8 @NiCo 2 S 4 heterogeneous nanosheets were directly grown on Nickel foamed (NF) through the hydrothermal+electrodeposition method to obtain a self-supporting electrode. Benefiting from its unique tremella-like structure, ultra-thin nanosheets, and the positive synergies between Co 9 S 8 and NiCo 2 S 4 , the prepared Co 9 S 8 @NiCo 2 S 4 @NF electrode presents a high specific capacity of 513 C g−1 (specific capacitance ~1026 F g−1) at 1 A g−1 with superior rate capability (62.8% capacitance retention rate at 10 A g−1). Furthermore, the fabricated Co 9 S 8 @NiCo 2 S 4 @NF//active carbon (AC) hybrid supercapacitor displays a high energy density of 30 Wh kg−1 at a power density of 731.8 W kg−1 and superior cycling stability. The results prove that the strategy of hydrothermal+electrodeposition is a very effective method for the preparation of energy storage and conversion materials with unique core-shell morphology. [Display omitted] • An integrated Co 9 S 8 @NiCo 2 S 4 @NF electrode is prepared. • Co 9 S 8 @NiCo 2 S 4 @NF presents a tremella-like porous structure. • The specific capacitance of Co 9 S 8 @NiCo 2 S 4 @NF can reach up to 1026 F g−1 at 1 A g−1. • A Co 9 S 8 @NiCo 2 S 4 @NF//AC hybrid supercapacitor is constructed. • The Co 9 S 8 @NiCo 2 S 4 @NF//AC displays a high energy density of 30 Wh kg−1. [ABSTRACT FROM AUTHOR]

Rational designing and preparing of electrode materials with desirable electrochemical performance by a simple, efficient and safe method is of great significance for electrochemical energy storage devices, but it is also challenging. In this study, ultrafine CoNi 2 S 4 nanowire arrays directly grown on carbon cloth (CC) are synthesized by sulfuration of Co–Ni hydroxide precursor. Benefiting from the high conductivity, the synergistic effect between Co and Ni ions and open self-supporting three-dimensional (3D) nanoarchitectures constructed by 1D CoNi 2 S 4 ultrafine nanowires, the as-obtained CoNi 2 S 4 @CC electrode exhibits excellent electrochemical capacitance performances: high specific capacitance of 1872 F g −1 at 1 A g −1and 1565 F g −1 at 5 A g−1. Meanwhile, a battery-supercapacitor hybrid (BSH) device is fabricated using the as-obtained CoNi 2 S 4 @CC as the positive electrode and porous carbon nanosheets (PCNS) derived from wood fungus as the negative electrode. The constructed BSH exhibits a high energy density of 37.2 Wh kg −1 at a power density of 0.75 kW kg−1, as well as a robust long-term cycling stability (97.6% capacitance retention after 10 000 charge-discharge cycles at a constant current density of 1 A g−1). These outstanding results verify CoNi 2 S 4 material has potential application in the energy storage field and it has been explored and expected to be the promising electrode materials for the supercapacitor. Image 1 • CoNi 2 S 4 @CC with 3D porous structure is prepared by a facile hydrothermal method. • 3D structure is constructed by 1D ultrafine nanowires vertically to the surface of CC. • The as-fabricated CoNi 2 S 4 @CCexhibited ultrahigh specific capacitance of 1872F g -1 at 1 A g -1. • CoNi 2 S 4 @CC//PCNS BSH device was constructed. • The CoNi 2 S 4 @CC//PCNS BSH device showed high energyand excellent cycling stability. [ABSTRACT FROM AUTHOR]

High-performance ternary cobalt-based metal oxides, especially ZnCo 2 O 4 , have attracted increasing attention as promising electrode materials for supercapacitors. However, there are still great challenges for the as-reported ZnCo 2 O 4 materials, such as self-aggregation during repeated discharging-charging process and low packing density. To tackle the above issues, it is envisaged as an efficient strategy to combine the advantages of both hierarchical porous micro/nanostructures and self-supporting electrode to fabricate a free-standing hierarchical micro/nanostructured ZnCo 2 O 4 electrode. Herein we propose an efficient and simple synthetic strategy for the controllable synthesis of self-supporting hierarchical porous cactus-like ZnCo 2 O 4 material directly grown on Ni-foam using a facile hydrothermal method with post-calcination treatment. Furthermore, a growth mechanism is also proposed. The as-prepared cactus-like ZnCo 2 O 4 material possesses unique structural merits, such as hierarchical porous structures, large specific surface area, robust structural stability, and strong connections between the substrate and the ZnCo 2 O 4 active material. The unique cactus-like ZnCo 2 O 4 film electrode displayed excellent electrochemical performance, including a high specific capacity of 1115.7 F g−1 at 1 A g−1 and remarkable long cycle stability with 80.8% capacity retention after 30,000 cycles. A practical asymmetric supercapacitor (ASC) device was assembled using cactus-like ZnCo 2 O 4 and active carbon, which showed an excellent energy density of 35.4 Wh kg−1 at high power density of 160.1 W kg−1 and superior cycle stability (62.5% capacity retention after 30,000 cycles at 1 A g−1). All these results show that such hierarchical porous ZnCo 2 O 4 micro/nanostructured films are a promising candidate for high-performance supercapacitors for energy storage application. [Display omitted] • 3D hierarchical porous cactus-like ZnCo 2 O 4 film is grown on Ni foam. • A growth mechanism of the 3D cactus-like ZnCo 2 O 4 film is proposed. • The cactus-like ZnCo 2 O 4 electrode shows 80.8% capacitance retention after 30,000 cycles at 5 A g−1. • The ZnCo 2 O 4 @NF//AC asymmetric supercapacitor exhibits an excellent energy density and power density. [ABSTRACT FROM AUTHOR]

• Quinone-enriched polymers (PDQs) are uniquely combined with reduced graphene oxides (rGOs) for assembling organic molecular electrodes (OMEs). • PDQ's extended π-conjugation system, substantial C O groups, and contorted structures result in excellent electrochemical properties, while strong π–π interactions with rGO enhance the cycling stability. • The as-prepared PDQ/rGO-0.3 delivers a specific electrochemical properties and an outstanding cycling stability. • The fabricated ASC exhibits good energy storage performance. In this study, quinone-enriched polymers (PDQs) are uniquely combined with reduced graphene oxides (rGOs) for assembling organic molecular electrodes (OMEs). The PDQ polymers are synthesized via a Schiff-base reaction involving 1,5-Diaminoanthraquinone (DAAQ) and 2,4,6-Triformylphloroglucinol (Tp). PDQ's extended π-conjugation system, substantial C O groups, and contorted structures result in excellent electrochemical properties, while strong π–π interactions with rGO enhance the cycling stability. The as-prepared PDQ/rGO-0.3 delivers a specific capacitance as high as 483.6 F g−1 at 5 mV s−1, with remarkable capacitance retentions (80 % at 100 mV s−1) and an outstanding cycling stability, where 87.8 % capacity retains after 10,000 cycles at a high current density of 5 A g−1. To verify actual energy storage performance of PDQ/rGO-0.3, an aqueous asymmetric supercapacitor (ASC) is assembled by employing 2,5-dihydroxy-1,4-benzoquinone-modified reduced graphite oxide (DHBQ/rGO) as another electrode, of which redox reaction occurs in a positive potential range. The assembled ASC displays a high energy density of 28.8 Wh kg−1 at a power density of 678 W kg−1, maintaining 98 % after 10,000 cycles in 1 M H 2 SO 4 aqueous electrolyte. To shed a light for practical use, a tandem configuration of two ASCs (PDQ/rGO-0.3//DHBQ/rGO) are demonstrated to power 46 LEDs effectively. Quinone-enriched polymers (PDQs) are uniquely combined with reduced graphene oxides (rGOs) to form organic molecular electrodes for use in all-carbon aqueous asymmetric supercapacitor (ASC). [Display omitted] [ABSTRACT FROM AUTHOR]

A redox-active organic molecular electrode is prepared for supercapacitors. Benzo[1,2-b:4,5-b']dithiophene-4,8-dione (BDTD), planar molecule with fused heteroaromatic structure, has been adsorbed on conductive reduced graphene oxide (rGO) by π–π interactions to form a 3D interconnected and functionalized xerogel (BDTD-rGO). Because the five-membered aromatic heterocycle is more electron-rich than the six-membered aromatic ring, which enlarges the electronic interaction between the BDTD molecule and the conjugated graphene network and accordingly reduce the solubility of BDTD molecule in electrolyte. As a result, the optimized BDTD-rGO electrodes achieve specific capacitance of 360 F g−1 at 1 A g−1, with ultra-long cycle life of 96.4% after 10,000 cycles, and even 80% after 50,000 cycles at 5 A g−1 in 1 M H 2 SO 4. Furthermore, the asymmetric supercapacitor (ASC), which is assembled by using the BDTD-rGO as the negative electrode and lamellar holey graphene hydrogel (LGH) as the positive electrode respectively, exhibits better energy storage performance. Image 1 • Reduced graphene oxide was non-covalently functionalized by organic molecules. • The BDTD-rGO exhibits an ultra-long cycle life (96.4% for 10,000 cycle). • The BDTD-rGO possesses an excellent specific capacitance of 360 F g−1 at 1 A g−1. • Negative and positive electrodes can generate potential self-matching behavior. • As-fabricated the asymmetric supercapacitor delivers a superior cyclic stability. [ABSTRACT FROM AUTHOR]

Provide more active sites and concise preparation is an effective technology in renewable energy storage sets. A soluble graphitic carbon nitride (SCN) nanosheets promoted two-dimensional nano electrochemical activity flake NiFe-LDH is successfully fabricated through electrostatic self-assembly, as a layer by layer high performance electrode (NiFe-LDH@SCN) for supercapacitor. The g-C 3 N 4 guarantees the effectiveness of the combination through the ζ-potential of g-C 3 N 4 flake (−19.5 mV) and NiFe-LDH flake (+15.6 mV), moreover, ensures the exposure of more active sites of NiFe-LDH. The optimized electrode shows an impressive specific capacitance of 1060.4 F g-1 at 1 A g-1 and remains 770.8 F g-1 at 10 A g-1. The fabricated hybrid supercapacitor (HSC) exhibits a magnificent energy density (up to 68.7 Wh kg-1) along with the power density of 827.5 W kg-1 in the wide voltage window of 1.7 V and a prominent long-term stability (83.3 % of capacitance retention even after 8000 cycles). Finally, two HSCs in series can light 40 LEDs. Hence, this work demonstrates the great potential of g-C 3 N 4 in developing high-performance LDH-based energy storage devices. [Display omitted] • The high performance electrode (NiFe-LDH@SCN) is fabricated through electrostatic self-assembly. • NiFe-LDH@SCN-32 electrode shows an impressive specific capacitance of 1060.4 F g-1 at 1 A g-1. • The NiFe-LDH@SCN-32//AC displays a high energy density of 68.7 Wh kg-1. • The capacitance retention is high up to 83.3 % after 8000 cycles. [ABSTRACT FROM AUTHOR]

• A fluorenone molecule electrode was reported, in which DHFO was anchored on GO to form hierarchical porous hydrogel. • The redox peak position of DHFO/rGO is located near 0.75 V, which is suitable for positive electrode in EES. • An ASC was assembled and delivered high energy density (28.57 Wh Kg−1), finally lighted 45 LED bulbs. Here, we report an organic molecule electrode for more efficient energy storage, in which 2,7-Dihydroxy-9-fluorenone (DHFO) molecules are anchored on interconnected and highly conductive graphene sheets by non-covalent π–π interactions. The optimal DHFO/rGO composite can reach a high specific capacitance of 412.3 F g−1 at scan rate of 5 mV s−1 in 1 mol L−1 H 2 SO 4 aqueous electrolyte with a satisfactory capacitive retention of 91% after 10,000 consecutive constant galvanostatic charge-discharge at current density of 5 A g−1. And it is worth noting that the Faraday current response peaks occurs within the positive potential range around 0.75 V, which is more suitable for positive electrode materials of supercapacitors with high performances. Additionally, charge storage mechanism and binding interactions of DHFO on graphene was evaluated based on the density functional theory (DFT) calculations. To match with the consequent positive electrode, AQ functionalized graphene (AQ/rGO) was prepared as negative electrode. Benefiting from the companionable match of two electrodes in structure, charge quantity and kinetics, the as-assembled asymmetrical supercapacitor (DHFO/rGO//AQ/rGO) delivers a maximum energy density of 28.57 Wh kg−1 along with 0.62 kW kg−1, and excellent cycle stability (82.3% specific capacitance retention after 10,000 cycling at 5 A g−1). Two tandem DHFO/rGO//AQ/rGO devices could light 45 LEDs. [Display omitted] [ABSTRACT FROM AUTHOR]

• BAQ and DHBQ are anchored on graphene to form organic molecules electrodes. • The BAQ (DHBQ)/rGO electrodes achieve capacitance all in excess of 400 F g−1 at 1 A g−1. • DFT calculations are employed to understand the experimental mechanism. • The two ASCs device in series easily lights 47 red light-emitting diodes compounding in parallel. Organic molecules electrodes with high electrochemical reversibility has enormous potential in energy storage. Here, benz[a]anthracene-7, 12-quinone (BAQ) and 2, 5-dihydroxy-p-benzoquinone (DHBQ) are anchored on reduced graphene oxide (rGO) [BAQ (DHBQ)/rGO] by non-convent method to form the porous 3D dry aerogels. The optimal BAQ (DHBQ)/rGO electrode materials display capacitance all in excess of 400 F g−1 at current density of 1 A g−1 and an excellent rate capability in 1 M H 2 SO 4 electrolyte. And BAQ/rGO and DHBQ/rGO are used respectively as the negative and positive electrode to fabricate the asymmetric supercapacitor (ASC), which achieves high energy density of 30.33 Wh kg−1 with power density of 802.9 W kg−1. Finally, 47 light-emitting diode (LED) bulbs aligned in a 'NWNU' shape are lit by two ASCs device in series, demonstrating its outstanding energy storage performance. Moreover, density functional theory (DFT) calculations are employed to understand the adsorption orientations, binding interactions and charge storage mechanism of BAQ on rGO surface, elucidating the superior electrochemical performance of the tested organic molecule electrode. In short, quinones non-covalently modified graphene is a promising and effective strategy for energy storage devices in future. [ABSTRACT FROM AUTHOR]