Functional mesoporous materials have gained tremendous attention due to their distinctive properties and potential applications. In recent decades, the self-assembly of micelles and framework precursors into mesostructures on the liquid−solid, liquid−liquid, and gas−liquid interface has been explored in the construction of functional mesoporous materials with diverse compositions, morphologies, mesostructures, and pore sizes. Compared with the one-phase solution synthetic approach, the introduction of a two-phase interface in the synthetic system changes self-assembly behaviors between micelles and framework species, leading to the possibility for the on-demand fabrication of unique mesoporous architectures. In addition, controlling the interfacial tension is critical to manipulate the self-assembly process for precise synthesis. In particular, recent breakthroughs based on the concept of the "monomicelles" assembly mechanism are very promising and interesting for the synthesis of functional mesoporous materials with the precise control. In this review, we highlight the synthetic strategies, principles, and interface engineering at the macroscale, microscale, and nanoscale for oriented interfacial assembly of functional mesoporous materials over the past 10 years. The potential applications in various fields, including adsorption, separation, sensors, catalysis, energy storage, solar cells, and biomedicine, are discussed. Finally, we also propose the remaining challenges, possible directions, and opportunities in this field for the future outlook.

Iridium (Ir)-based electrocatalysts are widely explored as benchmarks for acidic oxygen evolution reactions (OERs). However, further enhancing their catalytic activity remains challenging due to the difficulty in identifying active species and unfavorable architectures. In this work, we synthesized ultrathin Ir-IrO x /C nanosheets with ordered interlayer space for enhanced OER by a nanoconfined self-assembly strategy, employing block copolymer formed stable end-merged lamellar micelles. The interlayer distance of the prepared Ir-IrO x /C nanosheets was well controlled at ∼20 nm and Ir-IrO x nanoparticles (∼2 nm) were uniformly distributed within the nanosheets. Importantly, the fabricated Ir-IrO x /C electrocatalysts display one of the lowest overpotential (η) of 198 mV at 10 mA cm −2 geo during OER in an acid medium, benefiting from their features of mixed-valence states, rich electrophilic oxygen species (O (II-δ)− ), and favorable mesostructured architectures. Both experimental and computational results reveal that the mixed valence and O (II-δ)− moieties of the 2D mesoporous Ir-IrO x /C catalysts with a shortened Ir−O (II-δ)− bond (1.91 Å) is the key active species for the enhancement of OER by balancing the adsorption free energy of oxygen-containing intermediates. This strategy thus opens an avenue for designing high performance 2D ordered mesoporous electrocatalysts through a nanoconfined selfassembly strategy for water oxidation and beyond.

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