Mesoporous carbons hold a privileged position in the fields of catalysis, adsorption, and energy storage due to their high surface areas and naturally low density. Yet despite their immense potential, independent control over each architectural parameter (e.g., pore and wall dimensions) has eluded researchers due to a traditional reliance upon equilibration-based preparations. For micelle templates, the equilibration size is determined in part by the solution conditions. Should the solution conditions change, micelles can likewise respond by changing their equilibrium size and or morphology. Despite the immense popularity of equilibration-based micelle techniques, none have yet demonstrated sample series with constant template diameter and variable wall thickness. In contrast, persistent micelle templates (PMTs) are based off kinetically trapped micelles with arrested chain exchange kinetics. Such micelles do not change size despite changing solution conditions through increased material loadings. Prior PMT demonstrations required a rapid thermal cross-linking step which is not compatible with slow cross-linking carbon chemistries. Thus, we have developed a new modality of micelle persistence, glassy-PMT, which relies on micelles with an immobilized glassy core for greatly enhanced micelle persistence that is compatible with the slowly cross-linking carbon chemistries. We show that these glassy micelles enable the preparation of a carbon material series with constant average template diameter and variable wall thickness. Furthermore, the robust nature of these micelles is highlighted with direct TEM measurements which show the average template diameter to be commensurate with measurements after use as templates, providing the most direct evidence to-date for the PMT mechanism.

Tailored mesoporous carbons enabled by glassy persistent micelles

ACS Spring Meeting 2021

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