Metallic periodic structures provide unique optical and photonic coupling effects. However, geometrically precise control of periodic structure is particularly challenging when studying scale at few nanometer. Here, a new class of highly ordered silver plasmonic supercrystals is successfully synthesized by means of a nanocasting process using ordered mesoporous silica as template. During the nanocasting via a chemical reduction, the diffusibility, viscosity, and strength of the reducing agents have an important influence on the formation of ordered superstructures. The silver superstructures demonstrate an excellent structural stability even after removing the silica template and a small nanogap of less than ≈2 nm between nanoparticles, which are very vital for light–matter coupling, giving rise to plasmonic hot spots. The silver plasmonic supercrystals exhibit an ultrahigh Raman enhancement with an average enhancement factor of ≈10⁹ and an ultralow detection limit down to ≈0.1 × 10⁻¹⁵m for diverse chemical and biological molecules. This novel template strategy to fabricate periodic plasmonic nanostructures can lead to a new class of plasmonic nanostructures and open extraordinary potentials for diverse applications.

An ordered mesoporous WO₃ material with a highly crystalline framework was synthesized by using amphiphilic poly(ethylene oxide)-b-polystyrene (PEO-b-PS) diblock copolymers as a structure-directing agent through a solvent-evaporation-induced self-assembly method combined with a simple template-carbonization strategy. The obtained mesoporous WO₃ materials have a large uniform mesopore size (ca. 10.9 nm) and a high surface area (ca. 121 m² g⁻¹). The mesoporous WO₃-based H₂S gas sensor shows an excellent performance for H₂S sensing at low concentration (0.25 ppm) with fast response (2 s) and recovery (38 s). The high mesoporosity and continuous crystalline framework are responsible for the excellent performance in H₂S sensing.

An ordered mesoporous WO₃ material with a highly crystalline framework was synthesized by using amphiphilic poly(ethylene oxide)-b-polystyrene (PEO-b-PS) diblock copolymers as a structure-directing agent through a solvent-evaporation-induced self-assembly method combined with a simple template-carbonization strategy. The obtained mesoporous WO₃ materials have a large uniform mesopore size (ca. 10.9 nm) and a high surface area (ca. 121 m² g⁻¹). The mesoporous WO₃-based H₂S gas sensor shows an excellent performance for H₂S sensing at low concentration (0.25 ppm) with fast response (2 s) and recovery (38 s). The high mesoporosity and continuous crystalline framework are responsible for the excellent performance in H₂S sensing.

Ordered mesoporous materials have inspired prominent research interest due to their unique properties and functionalities and potential applications in adsorption, separation, catalysis, sensors, drug delivery, energy conversion and storage, and so on. Thanks to continuous efforts over the past two decades, great achievements have been made in the synthesis and structural characterization of mesoporous materials. In this review, we summarize recent progresses in preparing ordered mesoporous materials from the viewpoint of interfacial assembly and engineering. Five interfacial assembly and synthesis are comprehensively highlighted, including liquid-solid interfacial assembly, gas-liquid interfacial assembly, liquid-liquid interfacial assembly, gas-solid interfacial synthesis, and solid-solid interfacial synthesis, basics about their synthesis pathways, princples and interface engineering strategies.

A controllable one-pot method to synthesize N-doped ordered mesoporous carbons (NMC) with a high N content by using dicyandiamide as a nitrogen source via an evaporation-induced self-assembly process is reported. In this synthesis, resol molecules can bridge the Pluronic F127 template and dicyandiamide via hydrogen bonding and electrostatic interactions. During thermosetting at 100 °C for formation of rigid phenolic resin and subsequent pyrolysis at 600 °C for carbonization, dicyandiamide provides closed N species while resol can form a stable framework, thus ensuring the successful synthesis of ordered N-doped mesoporous carbon. The obtained N-doped ordered mesoporous carbons possess tunable mesostructures (p6m and Imm symmetry) and pore size (3.1–17.6 nm), high surface area (494–586 m² g⁻¹), and high N content (up to 13.1 wt%). Ascribed to the unique feature of large surface area and high N contents, NMC materials show high CO₂ capture of 2.8–3.2 mmol g⁻¹ at 298 K and 1.0 bar, and exhibit good performance as the supercapacitor electrode with specific capacitances of 262 F g⁻¹ (in 1 M H₂SO₄) and 227 F g⁻¹ (in 6 M KOH) at a current density of 0.2 A g⁻¹.

A novel ligand-assisted assembly approach is demonstrated for the synthesis of thermally stable and large-pore ordered mesoporous titanium dioxide with a highly crystalline framework by using diblock copolymer poly(ethylene oxide)-b-polystyrene (PEO-b-PS) as a template and titanium isopropoxide (TIPO) as a precursor. Small-angle X-ray scattering, X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution scanning electron microscopy, and N₂-sorption measurements indicate that the obtained TiO₂ materials possess an ordered primary cubic mesostructure with large, uniform pore diameters of about 16.0 nm, and high Brunauer–Emmett–Teller surface areas of ∼112 m² g⁻¹, as well as high thermal stability (∼700 °C). High resolution TEM and wide-angle XRD measurements clearly illustrate the high crystallinity of the mesoporous titania with an anatase structure in the pore walls. It is worth mentioning that, in this process, in addition to tetrahydrofuran as a solvent, acetylacetone was employed as a coordination agent to avoid rapid hydrolysis of the titanium precursor. Additionally, stepped evaporation and heating processes were adopted to control the condensation rate and facilitate the assembly of the ordered mesostructure, and ensure the formation of fully polycrystalline anatase titania frameworks without collapse of the mesostructure. By employing the obtained mesoporous and crystallized TiO₂ as the photoanode in a dye-sensitized solar cell, a high power-conversion efficiency (5.45%) can be achieved in combination with the N719 dye, which shows that this mesoprous titania is a great potential candidate as a catalyst support for photonic-conversion applications.