Designing hard carbon microsphere structure via halogenation amination and oxidative polymerization reactions for sodium ion insertion mechanism investigation.

Hard carbon as a negative electrode material for sodium-ion batteries (SIBs) has great commercial potential and has been widely studied. The sodium-ion intercalation in graphite domains and the filling of closed pores in the low voltage platform region still remain a subject of controversy. We have successfully constructed hard carbon materials with a pseudo-graphitic structure by using polymerizable p-phenylenediamine and dichloromethane as carbon sources. This was achieved by a halogenated amination reaction and oxidative polymerization. It was found that the capacity of hard carbon materials mainly originates from intercalation into graphite domains. The study found that the prepared hard carbon could store 339.33 mAh g-1 of sodium in a reversible way at a current density of 25 mA g-1, and it had an initial coulomb efficiency of 80.23%. It even maintained a reversible sodium storage capacity of 125.53 mAh g-1 at a high current density of 12.8 A g-1. Based on the analysis of hard carbon structure and electrochemical performance, it was shown that the materials conform with an "adsorption-intercalation" mechanism for sodium storage.

Rapid Electrochemical Activation of V2 O3 @C Cathode for High-Performance Zinc-Ion Batteries in Water-in-Salt Electrolyte.

Aqueous Zn-ion batteries (ZIBs), with the advantages of low cost, high safety, and high capacity, have great potential for application in grid energy storage and wearable flexible devices. However, their commercial application is still restricted by their inferior long-term cycling stability, Zn dendrite formation, and the decomposition of aqueous electrolyte. In this study, a Zn|Zn(CF3 SO3 )2 +LiTFSI|V2 O3 @C cell is constructed to address the above issues. The V2 O3 @C electrode can be fully oxidized into amorphous V2 O5 @C simultaneously with Zn2+ and H2 O co-insertion. The cell delivers a high specific capacity of more than 240 mAh g-1 at 3 A g-1 , with extraordinary coulombic efficiency and capacity retention. The excellent electrochemical performances are attributed to synergistic effects between the V2 O3 @C electrode and the water-in-salt electrolyte with enhanced stability and improved interface reaction kinetics. Systematic improvements of this architecture indicate much promise for application.

Controllable growth of carbon nanosheets in the montmorillonite interlayers for high-rate and stable anode in lithium ion battery.

A novel insertable and pseudocapacitive Li+ ion material for highly ordered layered montmorillonite/carbon is explored in the present study. The commercially available protonated montmorillonite and 3,3'-diaminobenzidine act as starting materials to synthesize the layered material via hydrothermal intercalation, oxidative polymerization and carbonization. This method of preparing montmorillonite/carbon nanocomposite exhibits several advantages. To be specific, raw materials are low cost and naturally abundant; the montmorillonite can undergo proton exchange easily to form a permutable proton-type material, and the protons in the layered nanocomposite can be directly substituted by the polymerizable molecules (e.g., 3,3'-diaminobenzidine). Accordingly, a sheet-like montmorillonite/carbon layered nanocomposite is achieved with the carbon stacking on the montmorillonite substrate for the intercalation behavior. As revealed from the electrochemical results, montmorillonite/carbon nanocomposite can deliver a high reversible capacity of 1432 mA h g-1 at 50 mA g-1 and superior rate capacity of 920 mA h g-1 at 10 000 mA g-1 for the lithium ion battery. Furthermore, the full cell with LiFePO4 as cathode and montmorillonite/carbon as anode maintains 94% capacity retention over 50 cycles as well as high coulombic efficiency.

Intercalation of Carbon Nanosheet into Layered TiO2 Grain for Highly Interfacial Lithium Storage.

Interfacial energy storage contributes a new mechanism to the emergence of energy storage devices with not only a high-energy density of batteries but also a high-power density of capacitors. In this study, success was achieved in preparing a highly ordered two-dimensional (2D) carbon/TiO2 (C/TiO2) nanosheet composite using commercially available organic molecules with multifunctional groups and taking advantage of the wedge effects, oxidative polymerization, and carbonization. An experiment was conducted to validate the excellent performance of this 2D composite with respect to interfacial energy storage. The coin cell with 2D C/TiO2 nanosheet composite demonstrates a specific capacity of as high as 510 mAh g-1 and a high specific energy of 390.9 Wh kg-1 at a specific power of 75.9 W kg-1 with a current density of 0.1 A g-1, and it also remains 39.0 Wh kg-1 at a specific power of 8.2 kW kg-1 with a high current density of 12.8 A g-1. The excellent electrochemical performance can be attributed to the superior artificial interface capacitive Li+ storage capability, which would bridge the energy and power density gap between batteries and capacitors. Meanwhile, there are two varieties of carbon derivatives, 2D carbon nanosheet stacks and exfoliated carbon nanosheets, which can be obtained by wet-chemical etching and mechanical peeling. The experimental route is simple from commercially available raw materials, and it could be scalable at a low cost and large scale, which makes it suitable for application in various fields such as energy storage, nanocatalysis, sensors, and so on.

Two-Dimensional Layered Ultrathin Carbon/TiO2 Nanosheet Composites for Superior Pseudocapacitive Lithium Storage.

Intercalation of carbon nanosheets into two-dimensional (2D) inorganic materials could enhance their properties in terms of mechanics and electrochemistry, but sandwiching these two kinds of materials in an alternating sequence is a great challenge in synthesis. Herein, we report a novel strategy to construct TiO2 nanosheets into 2D pillar-layer architectures by employing benzidine molecular assembly as pillars. Then, 2D carbon/TiO2 nanosheet composite with a periodic interlayer distance of 1.1 nm was obtained following a polymerization and carbonization process. This method not only alleviates the strain arising from the torsion of binding during carbonization but also hinders the structural collapse of TiO2 due to the intercalation of the carbon layer by rational control of annealing conditions. The composite material possesses a large carbon/TiO2 interface, providing abundant active sites for ultrafast pseudocapacitive charge storage, thus displaying a superior high-rate performance with a specific capacity of 67.8 mAh g-1 at a current density of 12.8 A g-1 based on the total electrode and excellent cyclability with 87.4% capacity retention after 3000 cycles.