Zeolite-templated carbons (ZTCs) comprise a relatively recent material class synthesized via the chemical vapor deposition of a carbon-containing precursor on a zeolite template, followed by the removal of the template. We have developed a theoretical framework to generate a ZTC from any given zeolite crystal structure, which we show can successfully predict the structure of known ZTCs. We use our method to generate a library of computationally-synthesized ZTCs from a large database of known zeolites, which allows us to establish criteria for which zeolites can produce experimentally-accessible triply-periodic ZTCs and to demonstrate over ten new ZTCs that have never before been synthesized, greatly enlarging the number of suitable zeolite templates from the three that have been determined by experimental trial and error. We show that these ZTCs are best characterized by their carbon-decorated surfaces, and that the topology and symmetry of these surfaces can be described by a pair of interpenetrating labyrinth nets. Since such a pair of nets also describes a triply periodic minimal surface (TPMS), our results establish the relationship between ZTCs and schwarzites—carbon materials with negative Gaussian curvature (as opposed to fullerenes and nanotubes with positive curvature, and graphene with zero curvature) that resemble TPMSs—linking the formerly disparate research topics and demonstrating that schwarzites should no longer be thought of as purely hypothetical materials. In addition to the numerous applications for which ZTCs are already being developed, we anticipate that the ability to synthesize a set of ZTCs with well-defined and diverse pore topologies will allow these materials to serve as a research platform for understanding the structure-property relationships of broad categories of porous carbons.

Towards an experimentally-accessible library of carbon schwarzites via zeolite-templating

256th National Meeting (2018)

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