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Title: C2 adsorption in zeolites: in silico screening and sensitivity to molecular models

Abstract

Efficient separation of ethane and ethylene has been a long-standing challenge for the chemical industry. In this work, we use molecular modeling to identify zeolite and zeotype frameworks that have the potential to be the next-generation solution for the separation of these C2 compounds. Using two different united-atom versions of the transferable potentials for phase equilibria (TraPPE) force field, the zeolitic structures in the database of the International Zeolite Association are screened for the separation of ethane and ethylene. A detailed analysis, with regards to accessibility of favorable sites and sensitivity to molecular models (also considering the explicit-hydrogen TraPPE model for ethane), is carried out on the top-performing structures. This study provides insights on the performance and limitations of molecular models for predicting mixture adsorption in zeolites.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]
  1. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science
  2. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemistry and Chemical Theory Center
  3. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science and Dept. of Chemistry and Chemical Theory Center
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Contributing Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
OSTI Identifier:
1463264
Alternate Identifier(s):
OSTI ID: 1434156
Grant/Contract Number:  
SC0008688; FG02–17ER16362; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Molecular Systems Design & Engineering
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2058-9689
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING

Citation Formats

Shah, Mansi S., Fetisov, Evgenii O., Tsapatsis, Michael, and Siepmann, J. Ilja. C2 adsorption in zeolites: in silico screening and sensitivity to molecular models. United States: N. p., 2018. Web. doi:10.1039/C8ME00004B.
Shah, Mansi S., Fetisov, Evgenii O., Tsapatsis, Michael, & Siepmann, J. Ilja. C2 adsorption in zeolites: in silico screening and sensitivity to molecular models. United States. doi:10.1039/C8ME00004B.
Shah, Mansi S., Fetisov, Evgenii O., Tsapatsis, Michael, and Siepmann, J. Ilja. Tue . "C2 adsorption in zeolites: in silico screening and sensitivity to molecular models". United States. doi:10.1039/C8ME00004B. https://www.osti.gov/servlets/purl/1463264.
@article{osti_1463264,
title = {C2 adsorption in zeolites: in silico screening and sensitivity to molecular models},
author = {Shah, Mansi S. and Fetisov, Evgenii O. and Tsapatsis, Michael and Siepmann, J. Ilja},
abstractNote = {Efficient separation of ethane and ethylene has been a long-standing challenge for the chemical industry. In this work, we use molecular modeling to identify zeolite and zeotype frameworks that have the potential to be the next-generation solution for the separation of these C2 compounds. Using two different united-atom versions of the transferable potentials for phase equilibria (TraPPE) force field, the zeolitic structures in the database of the International Zeolite Association are screened for the separation of ethane and ethylene. A detailed analysis, with regards to accessibility of favorable sites and sensitivity to molecular models (also considering the explicit-hydrogen TraPPE model for ethane), is carried out on the top-performing structures. This study provides insights on the performance and limitations of molecular models for predicting mixture adsorption in zeolites.},
doi = {10.1039/C8ME00004B},
journal = {Molecular Systems Design & Engineering},
number = 4,
volume = 3,
place = {United States},
year = {2018},
month = {4}
}

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Works referenced in this record:

TraPPE-zeo: Transferable Potentials for Phase Equilibria Force Field for All-Silica Zeolites
journal, November 2013

  • Bai, Peng; Tsapatsis, Michael; Siepmann, J. Ilja
  • The Journal of Physical Chemistry C, Vol. 117, Issue 46
  • DOI: 10.1021/jp4074224

Introduction of π-Complexation into Porous Aromatic Framework for Highly Selective Adsorption of Ethylene over Ethane
journal, June 2014

  • Li, Baiyan; Zhang, Yiming; Krishna, Rajamani
  • Journal of the American Chemical Society, Vol. 136, Issue 24
  • DOI: 10.1021/ja502119z

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

New sorbents for olefin/paraffin separations by adsorption viaπ -complexation
journal, March 1995


Enhanced ethylene separation and plasticization resistance in polymer membranes incorporating metal–organic framework nanocrystals
journal, April 2016

  • Bachman, Jonathan E.; Smith, Zachary P.; Li, Tao
  • Nature Materials, Vol. 15, Issue 8
  • DOI: 10.1038/nmat4621

Hydrocarbon Separations in a Metal-Organic Framework with Open Iron(II) Coordination Sites
journal, March 2012


Large-Scale Computational Screening of Zeolites for Ethane/Ethene Separation
journal, August 2012

  • Kim, Jihan; Lin, Li-Chiang; Martin, Richard L.
  • Langmuir, Vol. 28, Issue 32
  • DOI: 10.1021/la302230z

Seven chemical separations to change the world
journal, April 2016

  • Sholl, David S.; Lively, Ryan P.
  • Nature, Vol. 532, Issue 7600
  • DOI: 10.1038/532435a

Pure and binary adsorption isotherms of ethylene and ethane on zeolite 5A
journal, October 2012


Light olefins/paraffins separation with 13X zeolite binderless beads
journal, September 2014


Mixture Adsorption Equilibria of Ethane and Ethylene on 13X Molecular Sieves
journal, November 1978

  • Danner, Ronald P.; Choi, Edwin C. F.
  • Industrial & Engineering Chemistry Fundamentals, Vol. 17, Issue 4
  • DOI: 10.1021/i160068a003

Transferable Potentials for Phase Equilibria. 3. Explicit-Hydrogen Description of Normal Alkanes
journal, June 1999

  • Chen, Bin; Siepmann, J. Ilja
  • The Journal of Physical Chemistry B, Vol. 103, Issue 25
  • DOI: 10.1021/jp990822m

Transferable Potentials for Phase Equilibria. 4. United-Atom Description of Linear and Branched Alkenes and Alkylbenzenes
journal, August 2000

  • Wick, Collin D.; Martin, Marcus G.; Siepmann, J. Ilja
  • The Journal of Physical Chemistry B, Vol. 104, Issue 33
  • DOI: 10.1021/jp001044x

PFG NMR self-diffusion of propylene in ITQ-29, CaA and NaCaA: Window size and cation effects
journal, January 2007


Structure Determination of Novel Aluminophosphate Synthesized Using Diethylamine as Structure Directing Agents
journal, December 2016

  • Chang, Shuai; Jo, Gyeong Cheol; Kim, Joong Hyun
  • Advanced Porous Materials, Vol. 4, Issue 3
  • DOI: 10.1166/apm.2016.1113

On the location and disorder of the tetrapropylammonium (TPA) ion in zeolite ZSM-5 with improved framework accuracy
journal, April 1987

  • van Koningsveld, H.; van Bekkum, H.; Jansen, J. C.
  • Acta Crystallographica Section B Structural Science, Vol. 43, Issue 2
  • DOI: 10.1107/S0108768187098173

Transferable potentials for phase equilibria. Improved united-atom description of ethane and ethylene
journal, June 2017

  • Shah, Mansi S.; Siepmann, J. Ilja; Tsapatsis, Michael
  • AIChE Journal, Vol. 63, Issue 11
  • DOI: 10.1002/aic.15816

High pressure adsorptive separation of ethylene and ethane on Na-ETS-10
journal, June 2011


Adsorption of ethane and ethylene on modified ETS-10
journal, August 2008


The monoclinic framework structure of zeolite H-ZSM-5. Comparison with the orthorhombic framework of as-synthesized ZSM-5
journal, April 1990


A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984

  • Nosé, Shuichi
  • The Journal of Chemical Physics, Vol. 81, Issue 1
  • DOI: 10.1063/1.447334

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

  • Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
  • The Journal of Chemical Physics, Vol. 132, Issue 15
  • DOI: 10.1063/1.3382344

Highly selective adsorption of ethylene over ethane in a MOF featuring the combination of open metal site and π-complexation
journal, January 2015

  • Zhang, Yiming; Li, Baiyan; Krishna, Rajamani
  • Chemical Communications, Vol. 51, Issue 13
  • DOI: 10.1039/C4CC09774B

Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases
journal, September 2007

  • VandeVondele, Joost; Hutter, Jürg
  • The Journal of Chemical Physics, Vol. 127, Issue 11
  • DOI: 10.1063/1.2770708

Nosé–Hoover chains: The canonical ensemble via continuous dynamics
journal, August 1992

  • Martyna, Glenn J.; Klein, Michael L.; Tuckerman, Mark
  • The Journal of Chemical Physics, Vol. 97, Issue 4
  • DOI: 10.1063/1.463940

A Novel Open-Framework Cobalt Phosphate Containing a Tetrahedrally Coordinated Cobalt(II) Center: CoPO4· 0.5 C2H10N2
journal, March 1994

  • Chen, Jiesheng; Natarajan, Srinivasan; Thomas, John Meurig
  • Angewandte Chemie International Edition in English, Vol. 33, Issue 6
  • DOI: 10.1002/anie.199406391

Adsorptive separation of light olefins from paraffins
journal, August 2007


Sorption isotherms of methane, ethane, ethene and carbon dioxide on NaX, NaY and Na-mordenite zeolites
journal, January 1995

  • Choudhary, Vasant R.; Mayadevi, S.; Singh, Anand Pal
  • Journal of the Chemical Society, Faraday Transactions, Vol. 91, Issue 17
  • DOI: 10.1039/ft9959102935

Identifying Optimal Zeolitic Sorbents for Sweetening of Highly Sour Natural Gas
journal, April 2016

  • Shah, Mansi S.; Tsapatsis, Michael; Siepmann, J. Ilja
  • Angewandte Chemie International Edition, Vol. 55, Issue 20
  • DOI: 10.1002/anie.201600612

Phase equilibria by simulation in the Gibbs ensemble: Alternative derivation, generalization and application to mixture and membrane equilibria
journal, March 1988


Adsorption of methane, ethane, ethylene, and carbon dioxide on silicalite-l
journal, November 1996


Ethane/Ethene Separation Turned on Its Head: Selective Ethane Adsorption on the Metal−Organic Framework ZIF-7 through a Gate-Opening Mechanism
journal, December 2010

  • Gücüyener, Canan; van den Bergh, Johan; Gascon, Jorge
  • Journal of the American Chemical Society, Vol. 132, Issue 50
  • DOI: 10.1021/ja1089765

Efficient purification of ethene by an ethane-trapping metal-organic framework
journal, October 2015

  • Liao, Pei-Qin; Zhang, Wei-Xiong; Zhang, Jie-Peng
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9697

Canonical dynamics: Equilibrium phase-space distributions
journal, March 1985


A database of new zeolite-like materials
journal, January 2011

  • Pophale, Ramdas; Cheeseman, Phillip A.; Deem, Michael W.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 27
  • DOI: 10.1039/c0cp02255a

Membrane-based ethylene/ethane separation: The upper bound and beyond
journal, August 2013

  • Rungta, Meha; Zhang, Chen; Koros, William J.
  • AIChE Journal, Vol. 59, Issue 9
  • DOI: 10.1002/aic.14105

Future Directions of Membrane Gas Separation Technology
journal, March 2002

  • Baker, Richard W.
  • Industrial & Engineering Chemistry Research, Vol. 41, Issue 6
  • DOI: 10.1021/ie0108088

Adsorption and diffusion properties of hydrocarbons in zeolites
journal, August 2007


Adsorption equilibria of hydrocarbons on highly dealuminated zeolites
journal, March 1986


Adsorption equilibria of CO2 and small hydrocarbons in AEI-, CHA-, STT-, and RRO-type siliceous zeolites
journal, December 2016


Synthesis and Crystal Structure of As-Synthesized and Calcined Pure Silica Zeolite ITQ-12
journal, August 2004

  • Yang, Xiaobo; Camblor, Miguel A.; Lee, Yongjae
  • Journal of the American Chemical Society, Vol. 126, Issue 33
  • DOI: 10.1021/ja0481474

Shape Selectivity in Adsorption on the All-Silica DD3R
journal, April 2000

  • Zhu, W.; Kapteijn, F.; Moulijn, J. A.
  • Langmuir, Vol. 16, Issue 7
  • DOI: 10.1021/la9914007

Light hydrocarbon sorption properties of pure silica Si-CHA and ITQ-3 and high silica ZSM-58
journal, January 2004


ITQ-12:  A Zeolite Having Temperature Dependent Adsorption Selectivity and Potential for Propene Separation
journal, July 2004

  • Olson, David H.; Yang, Xiaobo; Camblor, Miguel A.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 30
  • DOI: 10.1021/jp040216d

cp2k: atomistic simulations of condensed matter systems
journal, June 2013

  • Hutter, Jürg; Iannuzzi, Marcella; Schiffmann, Florian
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 4, Issue 1
  • DOI: 10.1002/wcms.1159