Abstract
We report a new type of structural transformation occurring in methane adsorbed in micropores. The observed methane structures are defined by probability distributions of molecular positions. The mechanism of the transformation has been modeled using Monte Carlo method. The transformation is totally determined by a reconstruction of the probability distribution functions of adsorbed molecules. The methane molecules have some freedom to move in the pore but most of the time they are confined to the positions around the high probability adsorption sites. The observed high-probability structures evolve as a function of temperature and pressure. The transformation is strongly discontinuous at low temperature and becomes continuous at high temperature. The mechanism of the transformation is influenced by a competition between different components of the interaction and the thermal energy. The methane structure represents a new state of matter, intermediate between solid and liquid.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 16243-16246 |
| Number of pages | 4 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 56 |
| Issue number | 51 |
| DOIs | |
| State | Published - Dec 18 2017 |
Funding
This work was supported by the Polish National Science Centre (NCN, grant no. 2015/17/B/ST8/00099). The calculations have been partially performed at the WCSS computer center of The Wroclaw University of Science and Technology, grant No. 33.
Keywords
- adsorption
- metal–organic frameworks (MOFs)
- methane
- molecular modeling
- structural transformation
ASJC Scopus subject areas
- Catalysis
- General Chemistry