Strong Coupling of MoS2 Nanosheets and Nitrogen‐Doped Graphene for High‐Performance Pseudocapacitance Lithium Storage

Layered material MoS₂ is widely applied as a promising anode for lithium‐ion batteries (LIBs). Herein, a scalable and facile dopamine‐assisted hydrothermal technique for the preparation of strongly coupled MoS₂ nanosheets and nitrogen‐doped graphene (MoS₂/N‐G) composite is developed. In this composite, the interconnected MoS₂ nanosheets are well wrapped onto the surface of graphene, forming a unique veil‐like architecture. Experimental results indicate that dopamine plays multiple roles in the synthesis: a binding agent to anchor and uniformly disperse MoS₂ nanosheets, a morphology promoter, and the precursor for in situ nitrogen doping during the self‐polymerization process. Density functional theory calculations further reveal that a strong interaction exists at the interface of MoS₂ nanosheets and nitrogen‐doped graphene, which facilitates the charge transfer in the hybrid system. When used as the anode for LIBs, the resulting MoS₂/N‐G composite electrode exhibits much higher and more stable Li‐ion storage capacity (e.g., 1102 mAh g^?1 at 100 mA g^?1) than that of MoS₂/G electrode without employing the dopamine linker. Significantly, it is also identified that the thin MoS₂ nanosheets display outstanding high‐rate capability due to surface‐dominated pseudocapacitance contribution.     

Self‐Organized Graphene Nanosheets with Corrugated,Ordered Tip Structures for High‐Performance Flexible Field Emission

Patterned reduced graphene oxide (rGO) films with vertically aligned tip structures are fabricated by a straightforward self‐assembly method. The size, uniformity of the patterns, and alignment of the tips are successfully controlled according to the concentration of a GO/octadecylamine (ODA)‐dispersed solution. The surface energy difference between the GO/ODA solution and a self‐assembled water droplet is a critical parameter for determining the pattern structure. Numerous rGO nanosheets are formed so as to be vertically aligned with respect to the substrate during film fabrication at GO concentrations below 2.0 g/L. These samples provide high field‐emission characteristics. The patterned rGO arrays are highly flexible with preservation of the field emission properties, even at large bending angles. This is attributed to the high crystallinity, emitter density, and good chemical stability of the rGO arrays, as well as the strong interactions between the rGO arrays and the substrate.     

A Dynamic Graphene Oxide Network Enables Spray Printing of Colloidal Gels for High‐Performance Micro‐Supercapacitors

Properly controlling the rheological properties of nanoparticle inks is crucial to their printability. Here, it is reported that colloidal gels containing a dynamic network of graphene oxide (GO) sheets can display unusual rheological properties after high‐rate shearing. When mixed with polyaniline nanofiber dispersions, the GO network not only facilitates the gelation process but also serves as an effective energy‐transmission network to allow fast structural recovery after the gel is deformed by high‐rate shearing. This extraordinary fast recovery phenomenon has made it possible to use the conventional air‐brush spray technique to print the gel with high‐throughput and high fidelity on nonplanar flexible surfaces. The as‐printed micro‐supercapacitors exhibit an areal capacitance 4–6 times higher than traditionally spray‐printed ones. This work highlights the hidden potential of 2D materials as functional yet highly efficient rheological enhancers to facilitate industrial processing of nanomaterial‐based devices.     

Hierarchical 3D All‐Carbon Composite Structure Modified with N‐Doped Graphene Quantum Dots for High‐Performance Flexible Supercapacitors

Flexible supercapacitors have shown enormous potential for portable electronic devices. Herein, hierarchical 3D all‐carbon electrode materials are prepared by assembling N‐doped graphene quantum dots (N‐GQDs) on carbonized MOF materials (cZIF‐8) interweaved with carbon nanotubes (CNTs) for flexible all‐solid‐state supercapacitors. In this ternary electrode, cZIF‐8 provides a large accessible surface area, CNTs act as the electrical conductive network, and N‐GQDs serve as highly pseudocapactive materials. Due to the synergistic effect and hierarchical assembly of these components, N‐GQD@cZIF‐8/CNT electrodes exhibit a high specific capacitance of 540 F g^?1 at 0.5 A g^?1 in a 1 m H₂SO₄ electrolyte and excellent cycle stability with 90.9% capacity retention over 8000 cycles. The assembled supercapacitor possesses an energy density of 18.75 Wh kg^?1 with a power density of 108.7 W kg^?1. Meanwhile, three supercapacitors connected in series can power light‐emitting diodes for 20 min. All‐solid‐state N‐GQD@cZIF‐8/CNT flexible supercapacitor exhibits an energy density of 14 Wh kg^?1 with a power density of 89.3 W kg^?1, while the capacitance retention after 5000 cycles reaches 82%. This work provides an effective way to construct novel electrode materials with high energy storage density as well as good cycling performance and power density for high‐performance energy storage devices via the rational design.     

High Performance of N‐Doped Graphene with Bubble‐like Textures for Supercapacitors

Nitrogen‐doped graphene (NG) with wrinkled and bubble‐like texture is fabricated by a thermal treatment. Especially, a novel sonication‐assisted pretreatment with nitric acid is used to further oxidize graphene oxide and its binding with melamine molecules. There are many bubble‐like nanoflakes with a dimension of about 10 nm appeared on the undulated graphene nanosheets. The bubble‐like texture provides more active sites for effective ion transport and reversible capacitive behavior. The specific surface area of NG (5.03 at% N) can reach up to 438.7 m² g^?1, and the NG electrode demonstrates high specific capacitance (481 F g^?1 at 1 A g^?1, four times higher than reduced graphene oxide electrode (127.5 F g^?1)), superior cycle stability (the capacitance retention of 98.9% in 2 m KOH and 99.2% in 1 m H₂SO₄ after 8000 cycles), and excellent energy density (42.8 Wh kg^?1 at power density of 500 W kg^?1 in 2 m KOH aqueous electrolyte). The results indicate the potential use of NG as graphene‐based electrode material for energy storage devices.     

Freestanding 3D Graphene–Nickel Encapsulated Nitrogen‐Rich Aligned Bamboo Like Carbon Nanotubes for High‐Performance Supercapacitors with Robust Cycle Stability

3D hierarchical structures are reported based on graphene–nickel encapsulated nitrogen‐rich aligned bamboo like carbon nanotubes, which show not only high‐performance supercapacitance behavior but also a great robust cyclic stability. A facile synthesis route is developed of 2D nickel oxide decorated functionalized graphene nanosheets (2D‐NiO‐f:GNSs) hybrids and 3D nitrogen doped bamboo‐shaped carbon nanotubes (NCNTs) vertically standing on the functionalized graphene nanosheets (3D‐NCNT@f:GNSs) by using a thermal decomposition method. The chemical reduction and morphology‐dependent electrochemical response are investigated. The enhanced specific capacitance of 3D‐NCNT@f:GNSs as compared to that of 2D‐NiO‐f:GNSs suggests the synergistic effects and indicates the importance of energy storage and superior long‐term cycling performance that are achieved. This 3D‐NCNT@f:GNSs hybrid shows a remarkable cycling stability with a maximum power density of 12.32 kW kg⁻¹ and maximum energy density of 109.13 Wh kg⁻¹ due to the good connection of NCNT and f:GNSs. This unique 3D nano network architecture enables the availability of large surface areas of NCNT, thus endowing the nanohybrids with high specific capacitance and excellent reusability.     

Plasma Treatment for Nitrogen‐Doped 3D Graphene Framework by a Conductive Matrix with Sulfur for High‐Performance Li–S Batteries

Carbon materials have received considerable attention as host cathode materials for sulfur in lithium–sulfur batteries; N‐doped carbon materials show particularly high electrocatalytic activity. Efforts are made to synthesize N‐doped carbon materials by introducing nitrogen‐rich sources followed by sintering or hydrothermal processes. In the present work, an in situ hollow cathode discharge plasma treatment method is used to prepare 3D porous frameworks based on N‐doped graphene as a potential conductive matrix material. The resulting N‐doped graphene is used to prepare a 3D porous framework with a S content of 90 wt% as a cathode in lithium–sulfur cells, which delivers a specific discharge capacity of 1186 mAh g^?1 at 0.1 C, a coulombic efficiency of 96% after 200 cycles, and a capacity retention of 578 mAh g^?1 at 1.0 C after 1000 cycles. The performance is attributed to the flexible 3D structure and clustering of pyridinic N‐dopants in graphene. The N‐doped graphene shows high electrochemical performance and the flexible 3D porous stable structure accommodates the considerable volume change of the active material during lithium insertion and extraction processes, improving the long‐term electrochemical performance.     

Controlled 3D Assembly of Graphene Sheets to Build Conductive,Chemically Selective and Shape‐Responsive Materials

Driven by the surface activity of graphene, electrically conductive elastomeric foams have been synthesized by the controlled reassembly of graphene sheets; from their initial stacked morphology, as found in graphite, to a percolating network of exfoliated sheets, defining hollow spheres. This network creates a template for the formation of composite foams, whose swelling behavior is sensitive to the composition of the solvent, and whose electrical resistance is sensitive to physical deformation. The self‐assembly of graphene sheets is driven thermodynamically, as graphite is found to act as a 2D surfactant and is spread at high‐energy interfaces. This spreading, or exfoliation, of graphite at an oil/water interface stabilizes water‐in‐oil emulsions, without the need for added surfactants or chemical modification of the graphene. Using a monomer such as butyl acrylate for the emulsion's oil phase, elastomeric foams are created by polymerizing the continuous oil phase. Removal of the aqueous phase then results in robust, conductive, porous, and inexpensive composites, with potential applications in energy storage, filtration, and sensing.