skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: What Are the Best Materials To Separate a Xenon/Krypton Mixture?

Abstract

Accelerating progress in the discovery and deployment of advanced nanoporous materials relies on chemical insight and structure property relationships for rational design. Because of the complexity of this problem, trial-and-error is heavily involved in the laboratory today. A cost-effective route to aid experimental materials discovery is to construct structure models of nanoporous materials in silico and use molecular simulations to rapidly test them and elucidate data-driven guidelines for rational design. For example, highly-tunable nanoporous materials have shown promise as adsorbents for separating an industrially relevant gaseous mixture of xenon and krypton. Here in this work, we characterize, screen, and analyze the Nanoporous Materials Genome, a database of ca. 670,000 porous material structures, for candidate adsorbents for xenon/krypton separations. For over half a million structures, the computational resources required for a brute-force screening using grand-canonical Monte Carlo simulations of Xe/Kr adsorption are prohibitive. To overcome the computational cost, we used a hybrid approach combining machine learning algorithms (random forests) with molecular simulations. We compared the results from our large-scale screening with simple pore models to rationalize the strong link between pore size and selectivity. With this insight, we then analyzed the anatomy of the binding sites of the most selective materials.more » These binding sites can be constructed from tubes, pockets, rings, or cages and are often composed of non-discrete chemical fragments. The complexity of these binding sites emphasizes the importance of high-throughput computational screenings to discover new materials. Interestingly, our screening study predicts that the two most selective materials in the database are an aluminophosphate zeolite analogue and a calcium based coordination network, both of which have already been synthesized but not yet tested for Xe/Kr separations.« less

Authors:
 [1];  [2];  [3];  [1];  [4]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Norwegian Univ. of Science and Technology, Trondheim (Norway)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Scientific Computing Group
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States). Nanoporous Materials Genome Center
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
National Energy Research Scientific Computing Center
OSTI Identifier:
1474401
Grant/Contract Number:  
FG02-12ER16362; SC0008688
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 12; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Simon, Cory M., Mercado, Rocio, Schnell, Sondre K., Smit, Berend, and Haranczyk, Maciej. What Are the Best Materials To Separate a Xenon/Krypton Mixture?. United States: N. p., 2015. Web. doi:10.1021/acs.chemmater.5b01475.
Simon, Cory M., Mercado, Rocio, Schnell, Sondre K., Smit, Berend, & Haranczyk, Maciej. What Are the Best Materials To Separate a Xenon/Krypton Mixture?. United States. doi:10.1021/acs.chemmater.5b01475.
Simon, Cory M., Mercado, Rocio, Schnell, Sondre K., Smit, Berend, and Haranczyk, Maciej. Tue . "What Are the Best Materials To Separate a Xenon/Krypton Mixture?". United States. doi:10.1021/acs.chemmater.5b01475. https://www.osti.gov/servlets/purl/1474401.
@article{osti_1474401,
title = {What Are the Best Materials To Separate a Xenon/Krypton Mixture?},
author = {Simon, Cory M. and Mercado, Rocio and Schnell, Sondre K. and Smit, Berend and Haranczyk, Maciej},
abstractNote = {Accelerating progress in the discovery and deployment of advanced nanoporous materials relies on chemical insight and structure property relationships for rational design. Because of the complexity of this problem, trial-and-error is heavily involved in the laboratory today. A cost-effective route to aid experimental materials discovery is to construct structure models of nanoporous materials in silico and use molecular simulations to rapidly test them and elucidate data-driven guidelines for rational design. For example, highly-tunable nanoporous materials have shown promise as adsorbents for separating an industrially relevant gaseous mixture of xenon and krypton. Here in this work, we characterize, screen, and analyze the Nanoporous Materials Genome, a database of ca. 670,000 porous material structures, for candidate adsorbents for xenon/krypton separations. For over half a million structures, the computational resources required for a brute-force screening using grand-canonical Monte Carlo simulations of Xe/Kr adsorption are prohibitive. To overcome the computational cost, we used a hybrid approach combining machine learning algorithms (random forests) with molecular simulations. We compared the results from our large-scale screening with simple pore models to rationalize the strong link between pore size and selectivity. With this insight, we then analyzed the anatomy of the binding sites of the most selective materials. These binding sites can be constructed from tubes, pockets, rings, or cages and are often composed of non-discrete chemical fragments. The complexity of these binding sites emphasizes the importance of high-throughput computational screenings to discover new materials. Interestingly, our screening study predicts that the two most selective materials in the database are an aluminophosphate zeolite analogue and a calcium based coordination network, both of which have already been synthesized but not yet tested for Xe/Kr separations.},
doi = {10.1021/acs.chemmater.5b01475},
journal = {Chemistry of Materials},
number = 12,
volume = 27,
place = {United States},
year = {2015},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 72 works
Citation information provided by
Web of Science

Save / Share:

Works referencing / citing this record:

Neon-Bearing Ammonium Metal Formates: Formation and Behaviour under Pressure
journal, September 2016


An In-Situ Neutron Diffraction and DFT Study of Hydrogen Adsorption in a Sodalite-Type Metal-Organic Framework, Cu-BTTri : An
journal, January 2019

  • Asgari, Mehrdad; Semino, Rocio; Schouwink, Pascal
  • European Journal of Inorganic Chemistry, Vol. 2019, Issue 8
  • DOI: 10.1002/ejic.201801253

Metal–organic framework with optimally selective xenon adsorption and separation
journal, June 2016

  • Banerjee, Debasis; Simon, Cory M.; Plonka, Anna M.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11831