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Title: Statistical mechanical model of gas adsorption in porous crystals with dynamic moieties

Abstract

Some nanoporous, crystalline materials possess dynamic constituents, for example, rotatable moieties. These moieties can undergo a conformation change in response to the adsorption of guest molecules, which qualitatively impacts adsorption behavior. Here, we pose and solve a statistical mechanical model of gas adsorption in a porous crystal whose cages share a common ligand that can adopt two distinct rotational conformations. Guest molecules incentivize the ligands to adopt a different rotational configuration than maintained in the empty host. Our model captures inflections, steps, and hysteresis that can arise in the adsorption isotherm as a signature of the rotating ligands. The insights disclosed by our simple model contribute a more intimate understanding of the response and consequence of rotating ligands integrated into porous materials to harness them for gas storage and separations, chemical sensing, drug delivery, catalysis, and nanoscale devices. Particularly, our model reveals design strategies to exploit these moving constituents and engineer improved adsorbents with intrinsic thermal management for pressure-swing adsorption processes.

Authors:
ORCiD logo [1];  [1];  [1];  [2]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Valais Ecole Polytechnique Federale de Lausanne (EPFL), Sion (Switzerland)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1388053
Grant/Contract Number:  
SC0001015
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 3; Related Information: CGS partners with University of California, Berkeley; University of California, Davis; Lawrence Berkeley National Laboratory; University of Minnesota; National Energy Technology Laboratory; Texas A&M University; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Simon, Cory M., Braun, Efrem, Carraro, Carlo, and Smit, Berend. Statistical mechanical model of gas adsorption in porous crystals with dynamic moieties. United States: N. p., 2017. Web. doi:10.1073/pnas.1613874114.
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Simon, Cory M., Braun, Efrem, Carraro, Carlo, & Smit, Berend. Statistical mechanical model of gas adsorption in porous crystals with dynamic moieties. United States. https://doi.org/10.1073/pnas.1613874114
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Simon, Cory M., Braun, Efrem, Carraro, Carlo, and Smit, Berend. Tue . "Statistical mechanical model of gas adsorption in porous crystals with dynamic moieties". United States. https://doi.org/10.1073/pnas.1613874114. https://www.osti.gov/servlets/purl/1388053.
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@article{osti_1388053,
title = {Statistical mechanical model of gas adsorption in porous crystals with dynamic moieties},
author = {Simon, Cory M. and Braun, Efrem and Carraro, Carlo and Smit, Berend},
abstractNote = {Some nanoporous, crystalline materials possess dynamic constituents, for example, rotatable moieties. These moieties can undergo a conformation change in response to the adsorption of guest molecules, which qualitatively impacts adsorption behavior. Here, we pose and solve a statistical mechanical model of gas adsorption in a porous crystal whose cages share a common ligand that can adopt two distinct rotational conformations. Guest molecules incentivize the ligands to adopt a different rotational configuration than maintained in the empty host. Our model captures inflections, steps, and hysteresis that can arise in the adsorption isotherm as a signature of the rotating ligands. The insights disclosed by our simple model contribute a more intimate understanding of the response and consequence of rotating ligands integrated into porous materials to harness them for gas storage and separations, chemical sensing, drug delivery, catalysis, and nanoscale devices. Particularly, our model reveals design strategies to exploit these moving constituents and engineer improved adsorbents with intrinsic thermal management for pressure-swing adsorption processes.},
doi = {10.1073/pnas.1613874114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 3,
volume = 114,
place = {United States},
year = {2017},
month = {1}
}
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