Sodium‐ion batteries (SIBs) have gained tremendous interest for grid scale energy storage system and power energy batteries. However, the current researches of anode for SIBs still face the critical issues of low areal capacity, limited cycle life, and low initial coulombic efficiency for practical application perspective. To solve this issue, a kind of hierarchical 3D carbon‐networks/Fe7S8/graphene (CFG) is designed and synthesized as freestanding anode, which is constructed with Fe7S8 microparticles well‐welded on 3D‐crosslinked carbon‐networks and embedded in highly conductive graphene film, via a facile and scalable synthetic method. The as‐prepared freestanding electrode CFG represents high areal capacity (2.12 mAh cm−2 at 0.25 mA cm−2) and excellent cycle stability of 5000 cycles (0.0095% capacity decay per cycle). The assembled all‐flexible sodium‐ion battery delivers remarkable performance (high areal capacity of 1.42 mAh cm−2 at 0.3 mA cm−2 and superior energy density of 144 Wh kg−1), which are very close to the requirement of practical application. This work not only enlightens the material design and electrode engineering, but also provides a new kind of freestanding high energy density anode with great potential application prospective for SIBs.

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Functionalized porous carbon materials with hierarchical structure and developed porosity coming from natural and renewable biomass have been attracting tremendous attention recently. In this work, we present a facile and scalable method to synthesize MnO2 loaded carbonaceous aerogel (MnO2@CA) composites via the hydrothermal carbonaceous (HTC) process. We employ two reaction systems of the mixed metal ion precursors to study the optimal selective adsorption and further reaction of MnO2 precursor on CA. Our experimental results show that the system containing KMnO4 and Na2S2O3·5H2O exhibits better electrochemical properties compared with the reaction system of MnSO4·H2O and (NH4)2S2O8. For the former, the obtained MnO2@CA displays the specific capacitance of 123.5 F·g(-1). The enhanced supercapacitance of MnO2@CA nanocomposites could be ascribed to both electrochemical contributions of the loaded MnO2 nanoparticles and the porous structure of three-dimensional carbonaceous aerogels. This study not only indicates that it is vital for the reaction systems to match with porous carbonaceous materials, but also offers a new fabrication strategy to prepare lightweight and high-performance materials that can be used in energy storage devices.

In order to induce magnetism in two-dimensional semiconductors for their applications in spintronic devices and novel chemical and electronic properties of semiconducting phosphorene, the geometrical structure, electronic and magnetic properties of doped phosphorene monolayers with a series of nonmetal atoms, including H, F, Cl, Br, I, B, C, Si, N, As, O, S and Se, were systematically investigated using first-principles calculations. The results show that although the substitutional doping of H, F, Cl, Br, I, B, N, O, S or Se results in large structural deformation at the doping sites of phosphorene monolayers, all neutral nonmetal atom doped systems are stable. The calculated formation energies reveal that the substitutional doping of numerous nonmetal atoms in phosphorene monolayer are possible under appropriate experimental conditions, and the charged dopants C(-), Si(-), S(+) and Se(+) are stable. Moreover, the substitutional doping of H, F, Cl, Br, I, B, N, As, C(-), Si(-), S(+) or Se(+) cannot induce magnetism in phosphorene monolayer due to the saturation or pairing of valence electrons of dopant and its neighboring P atoms, whereas ground states of neutral C, Si, O, S or Se doped systems are magnetic due to the appearance of an unpaired valence electron of C and Si or the formation of a nonbonding 3p electron of a neighboring P atom around O, S and Se. Furthermore, the magnetic coupling between the moments induced by two Si, O, S or Se are long-range anti-ferromagnetic and the coupling can be attributed to the hybridization interaction involving polarized electrons, whereas the coupling between the moments induced by two C is weak.

Bismuth-based materials have attracted increasing attention in the research field of sodium/potassium-ion batteries owing to the high theoretical capacity. Unfortunately, the large volume variation and poor electrical conductivity limit their electrochemical performance and applications. Herein, we report a composite of heterostructured Bi 2 S 3 /MoS 2 encapsulated in nitrogen-doped carbon shell (BMS@NC) obtained by a solvothermal reaction as a novel anode material for sodium/potassium-ion batteries. The coating of the carbon layer could effectively relieve structural strains stemmed from the large volume change and improve electrical conductivity. More importantly, by skillfully constructing the heterostructure, an internal electric field formed on the heterointerface provides a rapid diffusion of ion and charge. As a consequence, the BMS@NC composite showed an excellent electrochemical performance for both sodium-ion batteries (a capacity of 381.5 mA h g −1 achieved at a current density of 5.0 A g −1 and 412 mA h g −1 at 0.5 A g −1 after 400 cycles) and potassium-ion batteries (a high specific capacity of 382.8 mA h g −1 achieved after 100 cycles at 0.1 A g −1 ). The design of the Bi 2 S 3 /MoS 2 heterostructure provides an effective strategy to develop energy storage materials with good electrochemical properties.

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