We describe a versatile and scalable strategy toward long-range and periodically ordered mesoporous alumina (AlO) structures by evaporation-induced self-assembly of a structure-directing ABA triblock copolymer (F127) mixed with aluminum tri--butoxide-derived sol additive. We found that the separate preparation of the alkoxide sol-gel reaction before mixing with the block copolymer enabled access to a relatively unexplored parameter space of copolymer-to-additive composition, acid-to-metal molar ratio, and solvent, yielding ordered mesophases of two-dimensional (2D) lamellar, hexagonal cylinder, and 3D cage-like cubic lattices, as well as multiscale hierarchical ordered structures from spinodal decomposition-induced macro- and mesophase separation. Thermal annealing in air at 900 °C yielded well-ordered mesoporous crystalline γ-AlO structures and hierarchically porous γ-AlO with 3D interconnected macroscale and ordered mesoscale pore networks. The ordered AlO structures exhibited tunable pore sizes in three different length scales, <2 nm (micropore), 2-11 nm (mesopore), and 1-5 μm (macropore), as well as high surface areas and pore volumes of up to 305 m/g and 0.33 cm/g, respectively. Moreover, the resultant mesoporous AlO demonstrated enhanced adsorption capacities of carbon dioxide and Congo red dye. Such hierarchically ordered mesoporous AlO are well-suited for green environmental solutions and urban sustainability applications, for example, high-temperature solid adsorbents and catalyst supports for carbon dioxide sequestration, fuel cells, and wastewater separation treatments.

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http://dx.doi.org/10.1021/acsami.1c06151DOI Listing

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