Two-dimensional materials, especially the newly emerging MXene, have attracted numerous interests in the fields of energy conversion/storage and electromagnetic shielding/absorption. However, the inherently inevitable aggregation and absence of magnetic loss of MXene considerably limit its electromagnetic absorption application. The introduction of magnetic component and favorable structural engineering are the alternatives to improve the microwave absorption (MA) performance. Herein, we report a spheroidization strategy to assemble double-shell MXene@Ni microspheres, where the commonly lamellar MXene are reshaped into three-dimensional microspheres that provide the substrate for oriented growth of Ni nanospikes. Whereas this structural feature offers massive accessible active surfaces that effectively promote the dielectric loss ability, the introduction of magnetic Ni nanospikes enables the additional magnetic loss capacity. Benefiting from these merits, the synthesized 3D MXene@Ni microspheres exhibit superior MA performance with the minimum reflection loss value of −59.6 dB at an ultrathin thickness (∼1.5 mm) and effective absorption bandwidth of 4.48 GHz. Moreover, the electron holography results reveal that the high-density anisotropy magnetism plays an important role in the improvement of MA performance, which provides an insight for the design of MXene-based materials as high-efficient microwave absorbers.

Yolk-shell microspheres with magnetic Fe3O4 cores and hierarchical copper silicate shells have been successfully synthesized by combining the versatile sol-gel process and hydrothermal reaction. Various yolk-shell microspheres with different core size and shell thickness can be readily synthesized by varying the experimental conditions. Compared to pure Fe3O4, the as-synthesized yolk-shell microspheres exhibit significantly enhanced microwave absorption properties in terms of both the maximum reflection loss value and the absorption bandwidth. The maximum reflection loss value of these yolk-shell microspheres can reach -23.5 dB at 7 GHz with a thickness of 2 mm, and the absorption bandwidths with reflection loss lower than -10 dB are up to 10.4 GHz. Owing to the large specific surface area, high porosity, and synergistic effect of both the magnetic Fe3O4 cores and hierarchical copper silicate shells, these unique yolk-shell microspheres may have the potential as high-efficient absorbers for microwave absorption applications.

Double-shelled yolk–shell microspheres with Fe3O4 cores and SnO2 double shells have been successfully synthesized by combining the versatile sol–gel process and hydrothermal shell-by-shell deposition method. The as-synthesized double-shelled Fe3O4@SnO2 yolk–shell microspheres have uniform size, unique morphology, well-defined shells, favorable magnetization, large specific surface area, and high porosity and exhibit significantly enhanced microwave absorption properties in terms of both the maximum reflection loss value and the absorption bandwidth. The excellent microwave absorption properties of these microspheres may be attributed to the unique double-shelled yolk–shell structure and synergistic effect between the magnetic Fe3O4 cores and dielectric SnO2 shells.

A facile and efficient strategy for the synthesis of hierarchical yolk-shell microspheres with magnetic Fe3O4 cores and dielectric TiO2 shells has been developed. Various Fe3O4@TiO2 yolk-shell microspheres with different core sizes, interstitial void volumes, and shell thicknesses have been successfully synthesized by controlling the synthetic parameters. Moreover, the microwave absorption properties of these yolk-shell microspheres, such as the complex permittivity and permeability, were investigated. The electromagnetic data demonstrate that the as-synthesized Fe3O4@TiO2 yolk-shell microspheres exhibit significantly enhanced microwave absorption properties compared with pure Fe3O4 and our previously reported Fe3O4@TiO2 core-shell microspheres, which may result from the unique yolk-shell structure with a large surface area and high porosity, as well as synergistic effects between the functional Fe3O4 cores and TiO2 shells.

Oriented self-assembly between inorganic nanocrystals and surfactants is emerging as a route for obtaining new mesocrystalline semiconductors. However, the actual synthesis of mesoporous semiconductor mesocrystals with abundant surface sites is extremely difficult, and the corresponding new physical and chemical properties arising from such an intrinsic porous mesocrystalline nature, which is of fundamental importance for designing high-efficiency nanostructured devices, have been rarely explored and poorly understood. Herein, we report a simple evaporation-driven oriented assembly method to grow unprecedented olive-shaped mesoporous TiO2 mesocrystals (FDU-19) self-organized by ultrathin flake-like anatase nanocrystals (∼8 nm in thickness). The mesoporous mesocrystals FDU-19 exhibit an ultrahigh surface area (∼189 m2/g), large internal pore volume (0.56 cm3/g), and abundant defects (oxygen vacancies or unsaturated Ti3+ sites), inducing remarkable crystallite-interface reactivity. It is found that the mesocrystals FDU-19 can be easily fused in situ into mesoporous anatase single crystals (SC-FDU-19) by annealing in air. More significantly, by annealing in a vacuum (∼4.0 × 10–5 Pa), the mesocrystals experience an abrupt three-dimensional to two-dimensional structural transformation to form ultrathin anatase single-crystal nanosheets (NS-FDU-19, ∼8 nm in thickness) dominated by nearly 90% exposed reactive (001) facets. The balance between attraction and electrostatic repulsion is proposed to determine the resulting geometry and dimensionality. Dye-sensitized solar cells based on FDU-19 and SC-FDU-19 samples show ultrahigh photoconversion efficiencies of up to 11.6% and 11.3%, respectively, which are largely attributed to their intrinsic single-crystal nature as well as high porosity. This work gives new understanding of physical and chemical properties of mesoporous semiconductor mesocrystals and opens up a new pathway for designing various single-crystal semiconductors with desired mesostructures for applications in catalysis, sensors, drug delivery, optical devices, etc.