Superparamagnetic microspheres with an Fe3O4@SiO2 core and a perpendicularly aligned mesoporous SiO2 shell were synthesized through a surfactant-templating sol-gel approach. The microspheres possess high magnetization (53.3 emu/g), high surface area (365 m2/g), large pore volume (0.29 cm3/g), and uniform mesopore (2.3 nm). By using the unique core-shell microspheres with accessible large pores and excellent magnetic property, a fast removal of microcystins with high efficiency (>95%) can be achieved.

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 Im$ \bar 3 $m 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.

The self-assembly of small surfactants and Pluronic® amphiphilic copolymers has enabled the synthesis of a range of ordered mesoporous materials with high surface area, diverse compositions, variable pore structures and tunable pore sizes. It has recently been realized that non-Pluronic block copolymers can be used as robust templates for the synthesis of novel and high-performance mesoporous materials with crystalline frameworks, ultra-large pores, and abundant pore symmetries, which are not accessible using the Pluronic counterparts. In this review, we introduce the principle of self-assembly of block copolymers and their phase separations, and summarize recently developed synthetic methods and strategies for ordered mesoporous silicas, metal oxides, carbons and metals which have shown superior performances for applications in various fields, including solar cells, batteries, fuel cells, and sensors.

Ordered mesoporous materials (OMMs) have received increasing interest due to their uniform pore size, high surface area, various compositions and wide applications in energy conversion and storage, biomedicine and environmental remediation, etc. The soft templating synthesis using surfactants or amphiphilic block copolymers is the most efficient method to produce OMMs with tailorable pore structure and surface property. However, due to the limited choice of commercially available soft templates, the common OMMs usually show small pore size and amorphous (or semicrystalline) frameworks. Tailor-made amphiphilic block copolymers with controllable molecular weights and compositions have recently emerged as alternative soft templates for synthesis of new OMMs with many unique features including adjustable mesostructures and framework compositions, ultralarge pores, thick pore walls, high thermal stability and crystalline frameworks. In this Perspective, recent progresses and some new insights into the coassembly process about the synthesis of OMMs based on these tailor-made copolymers as templates are summarized, and typical newly developed synthesis methods and strategies are discussed in depth, including solvent evaporation induced aggregation, ligand-assisted coassembly, solvent evaporation induced micelle fusion-aggregation assembly, homopolymer assisted pore expanding and carbon-supported crystallization strategy. Then, the applications of the obtained large-pore OMMs in catalysis, sensor, energy conversion and storage, and biomedicine by loading large-size guest molecules (e.g., protein and RNA), precious metal nanoparticles and quantum dots, are discussed. At last, the outlook on the prospects and challenges of future research about the synthesis of large-pore OMMs by using tailor-made amphiphilic block copolymers are included.