Abstract
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 model from any given zeolite structure, which we show can successfully predict the structure of known ZTCs. We use our method to generate a library of ZTCs from all known zeolites, to establish criteria for which zeolites can produce experimentally accessible ZTCs, and to identify over 10 ZTCs that have never before been synthesized. We show that ZTCs partition space into two disjoint labyrinths that can be described by a pair of interpenetrating 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 that resemble TPMSs-linking the research topics and demonstrating that schwarzites should no longer be thought of as purely hypothetical materials.
| Original language | English |
|---|---|
| Pages (from-to) | E8116-E8124 |
| Journal | Proceedings of the National Academy of Sciences of the United States of America |
| Volume | 115 |
| Issue number | 35 |
| DOIs | |
| Publication status | Published - 1 Jan 2018 |
| Externally published | Yes |
Funding
ACKNOWLEDGMENTS. We thank the responders on the LAMMPS mailing list for eliminating bugs in the AIREBO force field implementation (Steven J. Plimpton, Axel Kohlmeyer, Markus Hoehnerbach, Cyril Falvo, and Richard Berger were particularly helpful), Ben Slater for helpful discussions on carbon allotropes and TPMSs, and Peter Boyd for helpful discussions on crystal topology. This research was supported as part of the Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC0001015. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract DE-AC02-05CH11231. Y.L. thanks the ShanghaiTech University Research Startup Fund and the high-performance computing platform of ShanghaiTech University for support. S.M.M. acknowledges funding by the Deutsche Forschungsge-meinschaft (DFG, Priority Program SPP 1570). S.B. acknowledges funding by the National Center of Competence in Research (NCCR) Materials’ Revolution: Computational Design and Discovery of Novel Materials (“MARVEL”) of the Swiss National Science Foundation (SNSF). R.M. acknowledges support from an NSF Graduate Research Fellowship under Grant DGE 1106400. I.A.B. thanks the European Commission for support under the Graphene Flagship program (Contract NECT-ICT-604391). B.S. acknowledges support from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant Agreement 666983, MaGic).
| Funders | Funder number |
|---|---|
| Deutsche Forschungsge-meinschaft | SPP 1570 |
| ShanghaiTech University Research Startup Fund | |
| US Department of Energy | |
| National Science Foundation | DGE 1106400 |
| Environmental Leadership Program | |
| Office of Science | DE-AC02-05CH11231 |
| Basic Energy Sciences | DE-SC0001015 |
| Horizon 2020 Framework Programme | 666983 |
| European Commission | 604391 |
| European Research Council | |
| Office of Energy | |
| Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung | |
| National Center of Competence in Research Quantum Science and Technology | |
| ShanghaiTech University |
Keywords
- Microporous carbon
- Schwarzite
- Template carbonization
- Triply periodic minimal surface
- Zeolite-templated carbon