The role of charge-matching in nanoporous materials formation

Centi, Alessia and Manning, Joseph R. H. and Srivastava, Vibha and van Meurs, Sandra and Patwardhan, Siddharth V. and Jorge, Miguel (2019) The role of charge-matching in nanoporous materials formation. Materials Horizons, 6 (5). pp. 1027-1033. ISSN 2051-6355

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    Abstract

    Unravelling the molecular-level mechanisms that lead to the formation of mesoscale-ordered porous materials is a crucial step towards the goal of computational material design. For silica templated by alkylamine surfactants, a mechanism based on hydrogen-bond interactions between neutral amines and neutral silicates in solution has been widely accepted by the materials science community, despite the lack of conclusive evidence to support it. We demonstrate, through a combination of experimental measurements and multi-scale modelling, that the so-called "neutral templating route" does not represent a viable description of the synthesis mechanism of hexagonal mesoporous silica (HMS), the earliest example of amine-templated porous silica. Instead, the mesoscale structure of the material is defined by charge-matching of ionic interactions between amines and silicates. This has profound implications for the synthesis of a wide range of templated porous materials, and may shed new light on developing sustainable and economical routes to high value porous materials.