Solvated Graphene Frameworks as High‐Performance Anodes for Lithium‐Ion Batteries

A solvent‐exchange approach for the preparation of solvated graphene frameworks as high‐performance anode materials for lithium‐ion batteries is reported. The mechanically strong graphene frameworks exhibit unique hierarchical solvated porous networks and can be directly used as electrodes with a significantly improved electrochemical performance compared to unsolvated graphene frameworks, including very high reversible capacities, excellent rate capabilities, and superior cycling stabilities.     

Fabrication of Fe‐Doped LiCoO2 Sandwich‐Like Nanocomposites as Excellent Performance Cathode Materials for Lithium‐Ion Batteries

In this article, the two‐layer sandwiched graphene@LiFe_0.2Co_0.8O₂ nanoparticles (SG@LFCO) have been prepared and investigated as high‐rate and long‐life cathode materials for rechargeable lithium‐ion batteries. The materials possess a high‐surface area (267.1 m² g^?1) and lots of void spaces. By combining various favorable conditions, such as Fe doping, coating graphene, and designing novel morphology, the as‐prepared materials deliver a specific capacity of 115 mAh g^?1 at 10 C. At the 0.1 C cycling rate, the capacity retention of 97.2 % is sustained after 250 cycles and a coulombic efficiency of around 97.6 % is obtained.     

Sucrose‐Assisted Loading of LiFePO4 Nanoparticles on Graphene for High‐Performance Lithium‐Ion Battery Cathodes

A simple approach for loading LiFePO₄ (LFP) nanoparticles on graphene (G) that could assemble amorphous LiFePO₄ nanoparticles into a stable, crystalline, graphene‐modified layered materials (G‐S‐LFP, S=sucrose) by using graphene as building block and sucrose as a linker has yet to be developed. On the basis of differential scanning calorimetric and transmission electron microscopy analysis of the samples from controlled experiment, a possible mechanism was proposed to explain the “linker” process of LFP and graphene with sucrose as the linker. The electrochemical properties of the samples as cathode material for lithium‐ion batteries were studied by cyclic voltammogrametry and galvanostatic methods. Results showed that G‐S‐LFP displayed superior lithium‐storage capability with current density changes randomly form 0.5 to 10 C. The significant improvement for rate and cycle performance could be attributed to the high conductivity of the graphene host, the high crystallinity, and the layered structure.     

One‐Pot Synthesis of Carbon‐Coated Nanostructured Iron Oxide on Few‐Layer Graphene for Lithium‐Ion Batteries

Nanostructure engineering has been demonstrated to improve the electrochemical performance of iron oxide based electrodes in Li‐ion batteries (LIBs). However, the synthesis of advanced functional materials often requires multiple steps. Herein, we present a facile one‐pot synthesis of carbon‐coated nanostructured iron oxide on few‐layer graphene through high‐pressure pyrolysis of ferrocene in the presence of pristine graphene. The ferrocene precursor supplies both iron and carbon to form the carbon‐coated iron oxide, while the graphene acts as a high‐surface‐area anchor to achieve small metal oxide nanoparticles. When evaluated as a negative‐electrode material for LIBs, our composite showed improved electrochemical performance compared to commercial iron oxide nanopowders, especially at fast charge/discharge rates.     

Monodisperse Sandwich‐Like Coupled Quasi‐Graphene Sheets Encapsulating Ni2P Nanoparticles for Enhanced Lithium‐Ion Batteries

In this report, sandwiched Ni₂P nanoparticles encapsulated by graphene sheets are first synthesized by directly encapsulating functional units in graphene sheets instead of fabricating separate graphene sheets and then immobilizing the functional components onto the generated surfaces. In this strategy, we use low‐cost, sustainable and environmentally friendly glucose as a carbon source and NiNH₄PO₄ ? H₂O nanosheets as sacrificial templates. This unique structure obtained here cannot only prevent the nanoparticles from aggregation or loss but also enhance the electronic conductivity compared to the independent nanoparticles. Furthermore, the novel sandwich‐like Ni₂P/C can be applied in plenty of fields, especially in electrical energy storage. In this paper, a series of electrochemical tests of the sandwich‐like Ni₂P/C are carried out, which demonstrate the excellent cyclic stability and rate capacity for lithium‐ion batteries.     

Reduced Graphene Oxide‐Supported TiO2 Fiber Bundles with Mesostructures as Anode Materials for Lithium‐Ion Batteries

Although the synthesis of mesoporous materials is well established, the preparation of TiO₂ fiber bundles with mesostructures, highly crystalline walls, and good thermal stability on the RGO nanosheets remains a challenge. Herein, a low‐cost and environmentally friendly hydrothermal route for the synthesis of RGO nanosheet‐supported anatase TiO₂ fiber bundles with dense mesostructures is used. These mesostructured TiO₂‐RGO materials are used for investigation of Li‐ion insertion properties, which show a reversible capacity of 235 mA h g^?1 at 200 mA g^?1 and 150 mA h g^?1 at 1000 mA g^?1 after 1000 cycles. The higher specific surface area of the new mesostructures and high conductive substrate (RGO nanosheets) result in excellent lithium storage performance, high‐rate performance, and strong cycling stability of the TiO₂‐RGO composites.     

Excellent Performance of Few‐Layer Borocarbonitrides as Anode Materials in Lithium‐Ion Batteries

Borocarbonitrides (B_xC_yN_z) with a graphene‐like structure exhibit a remarkable high lithium cyclability and current rate capability. The electrochemical performance of the B_xC_yN_z materials, synthesized by using a simple solid‐state synthesis route based on urea, was strongly dependent on the composition and surface area. Among the three compositions studied, the carbon‐rich compound B_0.15C_0.73N_0.12 with the highest surface area showed an exceptional stability (over 100 cycles) and rate capability over widely varying current density values (0.05–1 A g^?1). B_0.15C_0.73N_0.12 has a very high specific capacity of 710 mA h g^?1 at 0.05 A g^?1. With the inclusion of a suitable additive in the electrolyte, the specific capacity improved drastically, recording an impressive value of nearly 900 mA h g^?1 at 0.05 A g^?1. It is believed that the solid–electrolyte interphase (SEI) layer at the interface of B_xC_yN_z and electrolyte also plays a crucial role in the performance of the B_xC_yN_z .     

Electrophoretic Deposition of Binder‐Free MnO2/Graphene Films for Lithium‐Ion Batteries

Binder‐free, nano‐sized needlelike MnO₂ ‐submillimeter‐sized reduced graphene oxide (nMnO₂‐srGO ) hybrid films with abundant porous structures were fabricated through electrophoretic deposition and subsequent thermal annealing at 500 °C for 2 h. The as‐prepared hybrid films exhibit a unique hierarchical morphology, in which nMnO₂ with a diameter of 20—50 nm and a length of 300—500 nm is randomly anchored on both sides of srGO . When evaluated as binder‐free anodes for lithium‐ion half‐cell, the nMnO₂‐srGO composites with a content of 76.9 wt% MnO₂ deliver a high capacity of approximately 1652.2 mA •h•g⁻¹ at a current density of 0.1 A•g⁻¹ after 200 cycles. The high capacity remains at 616.8 mA •h•g⁻¹ (ca. 65.1% capacity retention) at a current density as high as 4 A•g⁻¹. The excellent electrochemical performance indicates that the nMnO₂‐srGO hybrid films could be a promising anode material for lithium ion batteries (LIBs ).     

2 D Manganese Vanadate Nanoflakes as High‐Performance Anode for Lithium‐Ion Batteries

Nanometer‐sized flakes of MnV₂O₆ were synthesized by a hydrothermal method. No surfactant, expensive metal salt, or alkali reagent was used. These MnV₂O₆ nanoflakes present a high discharge capacity of 768 mA h g^?1 at 200 mA g^?1, good rate capacity, and excellent cycling stability. Further investigation demonstrates that the nanoflake structure and the specific crystal structure make the prepared MnV₂O₆ a suitable material for lithium‐ion batteries.     

Facile Mechanochemical Synthesis of Nano SnO2/Graphene Composite from Coarse Metallic Sn and Graphite Oxide: An Outstanding Anode Material for Lithium‐Ion Batteries

A facile method for the large‐scale synthesis of SnO₂ nanocrystal/graphene composites by using coarse metallic Sn particles and cheap graphite oxide (GO) as raw materials is demonstrated. This method uses simple ball milling to realize a mechanochemical reaction between Sn particles and GO. After the reaction, the initial coarse Sn particles with sizes of 3–30 μm are converted to SnO₂ nanocrystals (approximately 4 nm) while GO is reduced to graphene. Composite with different grinding times (1 h 20 min, 2 h 20 min or 8 h 20 min, abbreviated to 1, 2 or 8 h below) and raw material ratios (Sn:GO, 1:2, 1:1, 2:1, w/w) are investigated by X‐ray diffraction, X‐ray photoelectron spectroscopy, field‐emission scanning electron microscopy and transmission electron microscopy. The as‐prepared SnO₂/graphene composite with a grinding time of 8 h and raw material ratio of 1:1 forms micrometer‐sized architected chips composed of composite sheets, and demonstrates a high tap density of 1.53 g cm^?3. By using such composites as anode material for LIBs, a high specific capacity of 891 mA h g^?1 is achieved even after 50 cycles at 100 mA g^?1.     

Electrospun V2O5 Nanostructures with Controllable Morphology as High‐Performance Cathode Materials for Lithium‐Ion Batteries

Porous V₂O₅ nanotubes, hierarchical V₂O₅ nanofibers, and single‐crystalline V₂O₅ nanobelts were controllably synthesized by using a simple electrospinning technique and subsequent annealing. The mechanism for the formation of these controllable structures was investigated. When tested as the cathode materials in lithium‐ion batteries (LIBs), the as‐formed V₂O₅ nanostructures exhibited a highly reversible capacity, excellent cycling performance, and good rate capacity. In particular, the porous V₂O₅ nanotubes provided short distances for Li⁺‐ion diffusion and large electrode–electrolyte contact areas for high Li⁺‐ion flux across the interface; Moreover, these nanotubes delivered a high power density of 40.2 kW kg^?1 whilst the energy density remained as high as 201 W h kg^?1, which, as one of the highest values measured on V₂O₅‐based cathode materials, could bridge the performance gap between batteries and supercapacitors. Moreover, to the best of our knowledge, this is the first preparation of single‐crystalline V₂O₅ nanobelts by using electrospinning techniques. Interestingly, the beneficial crystal orientation provided improved cycling stability for lithium intercalation. These results demonstrate that further improvement or optimization of electrochemical performance in transition‐metal‐oxide‐based electrode materials could be realized by the design of 1D nanostructures with unique morphologies.     

Core–Shell LiFePO4/Carbon‐Coated Reduced Graphene Oxide Hybrids for High‐Power Lithium‐Ion Battery Cathodes

Core‐shell carbon‐coated LiFePO₄ nanoparticles were hybridized with reduced graphene (rGO) for high‐power lithium‐ion battery cathodes. Spontaneous aggregation of hydrophobic graphene in aqueous solutions during the formation of composite materials was precluded by employing hydrophilic graphene oxide (GO) as starting templates. The fabrication of true nanoscale carbon‐coated LiFePO₄‐rGO (LFP/C‐rGO) hybrids were ascribed to three factors: 1) In‐situ polymerization of polypyrrole for constrained nanoparticle synthesis of LiFePO₄, 2) enhanced dispersion of conducting 2D networks endowed by colloidal stability of GO, and 3) intimate contact between active materials and rGO. The importance of conducting template dispersion was demonstrated by contrasting LFP/C‐rGO hybrids with LFP/C‐rGO composites in which agglomerated rGO solution was used as the starting templates. The fabricated hybrid cathodes showed superior rate capability and cyclability with rates from 0.1 to 60 C. This study demonstrated the synergistic combination of nanosizing with efficient conducting templates to afford facile Li⁺ ion and electron transport for high power applications.     

Hollow and Yolk‐Shell Iron Oxide Nanostructures on Few‐Layer Graphene in Li‐Ion Batteries

We report a simple and template‐free strategy for the synthesis of hollow and yolk‐shell iron oxide (FeO_x) nanostructures sandwiched between few‐layer graphene (FLG) sheets. The morphology and microstructure of this material are characterized in detail by X‐ray diffraction, X‐ray absorption near‐edge structure, X‐ray photoelectron spectroscopy, Raman spectroscopy, scanning and transmission electron microscopy. Its properties are evaluated as negative electrode material for Li‐ion batteries and compared with those of solid FeO_x/FLG and two commercial iron oxides. In all cases, the content of carbon in the electrode has a great influence on the performance. The use of pristine FLG improves the capacity retention and further enhancement is achieved with the hollow structure. For a low carbon loading of 18 wt. %, the presence of metallic iron in the hollow and yolk‐shell FeO_x/FLG composite significantly enhances the capacity retention, albeit with a relatively lower initial reversible capacity, retaining above 97 % after 120 cycles at 1000 mA g^?1 in the voltage range of 0.1–3.0 V.     

Superior Electrochemical Performance of Sulfur/Graphene Nanocomposite Material for High‐Capacity Lithium–Sulfur Batteries

Sulfur/graphene nanocomposite material has been prepared by incorporating sulfur into the graphene frameworks through a melting process. Field‐emission scanning electron microscope analysis shows a homogeneous distribution of sulfur in the graphene nanosheet matrix. The sulfur/graphene nanocomposite exhibits a super‐high lithium‐storage capacity of 1580 mAh g^?1 and a satisfactory cycling performance in lithium–sulfur cells. The enhancement of the reversible capacity and cycle life could be attributed to the flexible graphene nanosheet matrix, which acts as a conducting medium and a physical buffer to cushion the volume change of sulfur during the lithiation and delithiation process. Graphene‐based nanocomposites can significantly improve the electrochemical performance of lithium–sulfur batteries.     

Hydrothermal Synthesis of Nickel Oxide Nanosheets for Lithium‐Ion Batteries and Supercapacitors with Excellent Performance

Nickel oxide nanosheets have been successfully synthesized by a facile ethylene glycol mediated hydrothermal method. The morphology and crystal structure of the nickel oxide nanosheets were characterized by X‐ray diffraction, field‐emission SEM, and TEM. When applied as electrode materials for lithium‐ion batteries and supercapacitors, nickel oxide nanosheets exhibited a high, reversible lithium storage capacity of 1193 mA h g^?1 at a current density of 500 mA g^?1, an enhanced rate capability, and good cycling stability. Nickel oxide nanosheets also demonstrated a superior specific capacitance of 999 F g^?1 at a current density of 20 A g^?1 in supercapacitors.     

Synthesis and Exploration of Ladder‐Structured Large Aromatic Dianhydrides as Organic Cathodes for Rechargeable Lithium‐Ion Batteries

Compared to anode materials in Li‐ion batteries, the research on cathode materials is far behind, and their capacities are much smaller. Thus, in order to address these issues, we believe that organic conjugated materials could be a solution. In this study, we synthesized two non‐polymeric dianhydrides with large aromatic structures: NDA‐4N (naphthalenetetracarboxylic dianhydride with four nitrogen atoms) and PDA‐4N (perylenetetracarboxylic dianhydride with four nitrogen atoms). Their electrochemical properties have been investigated between 2.0 and 3.9 V (vs. Li⁺/Li). Benefiting from multi‐electron reactions, NDA‐4N and PDA‐4N could reversibly achieve 79.7 % and 92.3 %, respectively, of their theoretical capacity. Further cycling reveals that the organic compound with a relatively larger aromatic building block could achieve a better stability, as an obvious 36.5 % improvement of the capacity retention was obtained when the backbone was switched from naphthalene to perylene. This study proposes an opportunity to attain promising small‐molecule‐based cathode materials through tailoring organic structures.     

Biomass‐Derived Porous Carbon with Micropores and Small Mesopores for High‐Performance Lithium–Sulfur Batteries

Biomass‐derived porous carbon BPC‐700, incorporating micropores and small mesopores, was prepared through pyrolysis of banana peel followed by activation with KOH. A high specific BET surface area (2741 m² g^?1), large specific pore volume (1.23 cm³ g^?1), and well‐controlled pore size distribution (0.6–5.0 nm) were obtained and up to 65 wt % sulfur content could be loaded into the pores of the BPC‐700 sample. When the resultant C/S composite, BPC‐700‐S65, was used as the cathode of a Li–S battery, a large initial discharge capacity (ca. 1200 mAh g^?1) was obtained, indicating a good sulfur utilization rate. An excellent discharge capacity (590 mAh g^?1) was also achieved for BPC‐700‐S65 at the high current rate of 4 C (12.72 mA cm^?2), showing its extremely high rate capability. A reversible capacity of about 570 mAh g^?1 was achieved for BPC‐700‐S65 after 500 cycles at 1 C (3.18 mA cm^?2), indicating an outstanding cycling stability.