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2D Bi2O2Se has recently attracted widespread research interest due to its high electron mobility and good air stability with tunable bandgap. However, the direct and controllable growth of large-size, high-quality ultrathin Bi2O2Se with tunable electronic properties remains a great challenge. Here, an organic ion template-guided solution growth method, is developed using water as a solvent to efficiently obtain high-quality 2D Bi2O2Se. Significantly, the thicknesses and morphologies of 2D Bi2OxSe with various oxygen deficiencies; are also achieved. Optical spectroscopic results indicate that oxygen defects can dramatically tune the electronic properties of Bi2O2Se, such as work function, band gap, and energy-band positions. As a result, the optimized Bi2O2Se devices exhibit a high photoresponsivity of 842.91 A W−1, photo-detectivity of 8.18 × 1012 Jones under 532 nm laser, and electron mobility of 334.7 cm2 V−1 s−1. This work proposes a new green solution method to synthesize large-sized, high-quality Bi2O2Se with tunable electronic structures that can be extended for various applications and provides a new possibility of transfer-free large-scale device manufacturing. National Research Foundation (NRF) The work was supported by Fund of National Key Laboratory of Science and Technology on Advanced Composites in Special Environments (Grant No. 6142905192507), Shenzhen Science and Technology Plan Supported Project (Grant Nos. GXWD20201230155427003-20200821232246001, JCYJ20170413105844696). Z.L. acknowledges the financial support from Singapore National Research Foundation Competitive Research Program (Grant No. NRF-CRP22-2019-0007).

The cycling stability of high-sulfur-loading lithium–sulfur (Li–S) batteries remains a great challenge owing to the exaggerated shuttle problem and interface instability. Despite enormous efforts on design of advanced electrodes and electrolytes, the stability issue raised from current collectors has been rarely concerned. This study demonstrates that rationally designing a 3D carbonaceous macroporous current collector is an efficient and effective “two-in-one” strategy to improve the cycling stability of high-sulfur-loading Li–S batteries, which is highly versatile to enable various composite cathodes with sulfur loading >3.7 mAh cm−2. The best cycling performance can be achieved upon 950 cycles with a very low decay rate of 0.029%. Moreover, the origin of such a huge enhancement in cycling stability is ascribed to (1) the inhibition of electrochemical corrosion, which severely occurs on the typical Al foil and disables its long-term sustainability for charge transfer, and (2) the passivation of cathode surface. The role of the chemical resistivity against corrosion and favorable macroscopic porous structure is highlighted for exploiting novel current collectors toward exceptional cycling stability of high-sulfur-loading Li–S batteries.

The rational combination of conductive nanocarbon with sulfur leads to the formation of composite cathodes that can take full advantage of each building block; this is an effective way to construct cathode materials for lithium–sulfur (Li–S) batteries with high energy density. Generally, the areal sulfur-loading amount is less than 2.0 mg cm−2, resulting in a low areal capacity far below the acceptable value for practical applications. In this contribution, a hierarchical free-standing carbon nanotube (CNT)-S paper electrode with an ultrahigh sulfur-loading of 6.3 mg cm−2 is fabricated using a facile bottom–up strategy. In the CNT–S paper electrode, short multi-walled CNTs are employed as the short-range electrical conductive framework for sulfur accommodation, while the super-long CNTs serve as both the long-range conductive network and the intercrossed mechanical scaffold. An initial discharge capacity of 6.2 mA·h cm−2 (995 mA·h g−1), a 60% utilization of sulfur, and a slow cyclic fading rate of 0.20%/cycle within the initial 150 cycles at a low current density of 0.05 C are achieved. The areal capacity can be further increased to 15.1 mA·h cm−2 by stacking three CNT–S paper electrodes—resulting in an areal sulfur-loading of 17.3 mg cm−2—for the cathode of a Li–S cell. The as-obtained free-standing paper electrode are of low cost and provide high energy density, making them promising for flexible electronic devices based on Li–S batteries.

The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) play a decisive role for the efficiency of fuel cells and metal-air batteries. The nitrogen doped carbon materials with low cost and long durability are potential catalysts to replace precious metal catalyst for oxygen electrochemistry; however, the unexposed active sites induced by the bulk dopant atoms are hardly accessible and consequently scarcely contribute to the catalytic property. In this study, carbon nanotubes (CNTs) are selected as the platform to demonstrate the potential of full exposure of active sites' at the surface. Novel N-doped carbon coaxial nanocables with the pristine CNTs as the core and the N-doped carbon layers as the shell are proposed. The accessible and efficient utilization of the integrated nitrogen atoms enriched on the surface, together with the undestroyed intact inner walls, render the electrocatalyst much enhanced electrocatalytic activity and high electrical conductivity of 3.3 S cm(-1), therefore, N-doped nanocables afford higher oxygen reduction current, approximate to 51 mV positively shift onset potential, low peroxide generation, as well as lower overpotential and higher current for oxygen evoluation reaction.

The sp2-hybridized nanocarbon (e.g., carbon nanotubes (CNTs) and graphene) exhibits extraordinary mechanical strength and electrical conductivity but limited external accessible surface area and a small amount of pores, while nanostructured porous carbon affords a huge surface area and abundant pore structures but very poor electrical conductance. Herein the rational hybridization of the sp2 nanocarbon and nanostructured porous carbon into hierarchical all-carbon nanoarchitectures is demonstrated, with full inherited advantages of the component materials. The sp2 graphene/CNT interlinked networks give the composites good electrical conductivity and a robust framework, while the meso-/microporous carbon and the interlamellar compartment between the opposite graphene accommodate sulfur and polysulfides. The strong confinement induced by micro-/mesopores of all-carbon nanoarchitectures renders the transformation of S8 crystal into amorphous cyclo-S8 molecular clusters, restraining the shuttle phenomenon for high capacity retention of a lithium-sulfur cell. Therefore, the composite cathode with an ultrahigh specific capacity of 1121 mAh g−1 at 0.5 C, a favorable high-rate capability of 809 mAh g−1 at 10 C, a very low capacity decay of 0.12% per cycle, and an impressive cycling stability of 877 mAh g−1 after 150 cycles at 1 C. As sulfur loading increases from 50 wt% to 77 wt%, high capacities of 970, 914, and 613 mAh g−1 are still available at current densities of 0.5, 1, and 5 C, respectively. Based on the total mass of packaged devices, gravimetric energy density of GSH@APC-S//Li cell is expected to be 400 Wh kg−1 at a power density of 10 000 W kg−1, matching the level of engine driven systems.

The high-end applications of single-walled carbon nanotubes (SWCNTs) are hindered by the existence of large amount of impurities, especially the graphene layers encapsulating metal nanoparticles (metal@C NPs). The role of working metal catalysts during chemical vapor deposition (CVD) growth and post purifications by oxidation are not yet fully understood. Herein, the in situ monitoring the role of working metal catalyst NPs for ultrahigh purity SWCNTs by CVD growth and CO2 purifications is carried out in an online thermogravimetric reactor attached with a mass spectrometer. The growth of SWCNTs almost stops after the initial 2 min, then, the mass increase of the samples mainly originates from the metal@CNP formation. Therefore, high-purity SWCNTs (98.5 wt%) with few metal@CNPs can be available by 2 min CVD growth. Furthermore, CO2 oxidation of the SWCNTs is also investigated in a thermogravimetric reactor. The oxidation of graphene layers surrounding the metal NPs and the SWCNTs occurs during distinct temperature ranges, which is further demonstrated by the significant differences among their oxidation activation energies. Ultrahigh purity of SWNCT with a carbon content of 99.5 wt% can be available by a CO2-assited purification method. The in situ study of the CVD growth and CO2 oxidation of SWCNTs provides the real time information on the working catalyst during reaction and the reactivity information of metal@CNPs and SWCNTs under an oxidizing atmosphere. The success for the preparation of high-purity SWCNT lies in the efficient growth of SWCNTs with a low amount of nanocarbon impurities and partial oxidation of metal@CNPs by catalytic CO2 oxidation with proper operation parameters.

The combination of one-dimensional and two-dimensional building blocks leads to the formation of hierarchical composites that can take full advantages of each kind of material, which is an effective way for the preparation of multifunctional materials with extraordinary properties. Among various building blocks, nanocarbons (e.g., carbon nanotubes and graphene) and layered double hydroxides (LDHs) are two of the most powerful materials that have been widely used in human life. This Feature Article presents a state-of-the-art review of hierarchical nanocomposites derived from nanocarbons and LDHs. The properties of nanocarbons, LDHs, as well as the combined nanocomposites, are described first. Then, efficient and effective fabrication methods for the hierarchical nanocomposites, including the reassembly of nanocarbons and LDHs, formation of LDHs on nanocarbons, and formation of nanocarbons on LDHs, are presented. The as-obtained nanocomposites derived form nanocarbons and LDHs exhibited excellent performance as multifunctional materials for their promising applications in energy storage, nanocomposites, catalysis, environmental protection, and drug delivery. The fabrication of LDH/carbon nanocomposites provides a novel method for the development of novel multifunctional nanocomposites based on the existing nanomaterials. However, knowledge of their assembly mechanism, robust and precise route for LDH/nanocarbon hybrid with well designed structure, and the relationship between structure, properties, and applications are still inadequate. A multidisciplinary approach from the scope of materials, physics, chemistry, engineering, and other application areas, is highly required for the development of this advanced functional composite materials.

Three-dimensional hierarchical nanocomposites consisting of one-dimensional carbon nanotubes (CNTs) and two-dimensional lamellar flakes (such as clay, layered double hydroxides) show unexpected properties for unique applications. To achieve a well-designed structure with a specific function, the uniform distribution of CNTs into the used matrix is a key issue. Here, it is shown that a hierarchical composite of single/double-walled CNTs interlinked with two-dimensional flakes can be constructed via in-situ CNT growth onto layered double hydroxide (LDH) flakes. Both the wall number and diameter of the CNTs and the composition of the flakes can be easily tuned by changing the proportion of the transition metal in the LDH flakes. Furthermore, a structure with continuously interlinked CNT layers alternating with lamellar flakes is obtained after compression. The hierarchical composite is demonstrated to be an excellent filler for strong polyimide films. This study indicates that LDH is an extraordinary catalyst for the fabrication of hierarchical composites with high-quality single/double-walled CNTs. The as-obtained CNTs/calcined LDHs nanocomposite is a novel structural platform for the design of mechanically robust materials, catalysts, ion-transportation, energy-conversion, and other applications.

Growth of aligned and uniform α-Fe2O3 nanowire (NW) arrays has been achieved by a vapor–solid process. The experimental conditions, such as type of substrate, local growth and geometrical environment, gas-flow rate, and growth temperature, under which the high density α-Fe2O3 NW arrays can be grown by a vapor–solid route via the tip-growth mechanism have been systematically investigated. The density of the α-Fe2O3 NWs can be enhanced by increasing the concentration of Ni atoms inside the alloy substrate. The synthesized temperature can be as low as 400 °C. Fe3O4 NWs can be produced by converting α-Fe2O3 NWs in a reducing atmosphere at 450 °C. The transformation of phase and structure have been observed by in situ transmission electron microscopy. The magnetic and field-emission properties of the NWs indicate their potential applications in nanodevices.