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Title: Molecular simulations of H2 adsorption in metal-porphyrin frameworks: A potential new material evaluation

Abstract

Path integral grand canonical Monte Carlo (PI-GCMC) simulations using standard force fields are typically carried out to calculate the adsorption of H2 in five metal-porphyrin frameworks (MPFs), a new class of metal organic framework (MOF)-type materials. These simulations are performed at 77 K and room temperature (300 K). The adsorption isotherms of H2 in IRMOF-1 and IRMOF-10 are also calculated as a comparison. All calculations indicate that all MPFs adsorbed a higher weight fraction of H2 than both IRMOF-1 and IRMOF-10, with one exception (MPF-2). The gravimetric hydrogen capacities are still well short of practical goals. The MPFs provide additional adsorption sites due to the porphyrin. A statistical mechanical lattice model predicts the adsorption well at room temperature. The prediction by this model reflected that a weight fraction of hydrogen of 6 wt. % adsorbed in pores of the size found in IRMOF-1 at ambient temperature and modest pressures required a binding energy of about 17 kJ/mole, which is consistent with other findings.

Authors:
 [1];  [2]
  1. Univ. of Delaware, Newark, DE (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
1564774
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Renewable and Sustainable Energy
Additional Journal Information:
Journal Volume: 3; Journal Issue: 5; Journal ID: ISSN 1941-7012
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN

Citation Formats

Xiong, Ruichang, and Keffer, David J. Molecular simulations of H2 adsorption in metal-porphyrin frameworks: A potential new material evaluation. United States: N. p., 2011. Web. doi:10.1063/1.3655373.
Xiong, Ruichang, & Keffer, David J. Molecular simulations of H2 adsorption in metal-porphyrin frameworks: A potential new material evaluation. United States. https://doi.org/10.1063/1.3655373
Xiong, Ruichang, and Keffer, David J. 2011. "Molecular simulations of H2 adsorption in metal-porphyrin frameworks: A potential new material evaluation". United States. https://doi.org/10.1063/1.3655373. https://www.osti.gov/servlets/purl/1564774.
@article{osti_1564774,
title = {Molecular simulations of H2 adsorption in metal-porphyrin frameworks: A potential new material evaluation},
author = {Xiong, Ruichang and Keffer, David J.},
abstractNote = {Path integral grand canonical Monte Carlo (PI-GCMC) simulations using standard force fields are typically carried out to calculate the adsorption of H2 in five metal-porphyrin frameworks (MPFs), a new class of metal organic framework (MOF)-type materials. These simulations are performed at 77 K and room temperature (300 K). The adsorption isotherms of H2 in IRMOF-1 and IRMOF-10 are also calculated as a comparison. All calculations indicate that all MPFs adsorbed a higher weight fraction of H2 than both IRMOF-1 and IRMOF-10, with one exception (MPF-2). The gravimetric hydrogen capacities are still well short of practical goals. The MPFs provide additional adsorption sites due to the porphyrin. A statistical mechanical lattice model predicts the adsorption well at room temperature. The prediction by this model reflected that a weight fraction of hydrogen of 6 wt. % adsorbed in pores of the size found in IRMOF-1 at ambient temperature and modest pressures required a binding energy of about 17 kJ/mole, which is consistent with other findings.},
doi = {10.1063/1.3655373},
url = {https://www.osti.gov/biblio/1564774}, journal = {Journal of Renewable and Sustainable Energy},
issn = {1941-7012},
number = 5,
volume = 3,
place = {United States},
year = {Wed Oct 19 00:00:00 EDT 2011},
month = {Wed Oct 19 00:00:00 EDT 2011}
}

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Cited by: 4 works
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Works referenced in this record:

Modelling of hydrogen adsorption in the metal organic framework MOF5
journal, October 2005


Storage of hydrogen in single-walled carbon nanotubes
journal, March 1997


Effects of Surface Area, Free Volume, and Heat of Adsorption on Hydrogen Uptake in Metal−Organic Frameworks
journal, April 2006


Adsorption in Porous Materials at High Pressure:  Theory and Experiment
journal, December 2002


Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids
journal, January 1996


Molecular simulation of adsorption sites of light gases in the metal-organic framework IRMOF-1
journal, December 2007


Hydrogen storage on superactivated carbon at refrigeration temperatures
journal, January 1989


Supermolecular Building Blocks (SBBs) for the Design and Synthesis of Highly Porous Metal-Organic Frameworks
journal, February 2008


Space-Time Approach to Non-Relativistic Quantum Mechanics
journal, April 1948


UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992


Significantly Enhanced Hydrogen Storage in Metal−Organic Frameworks via Spillover
journal, January 2006


Cover Picture
journal, March 2006


A functional zeolite analogue assembled from metalloporphyrins
journal, September 2002


Molecular Simulation of Carbon Dioxide/Methane/Hydrogen Mixture Adsorption in Metal−Organic Frameworks
journal, September 2006


Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage
journal, January 2002


DREIDING: a generic force field for molecular simulations
journal, December 1990


Optimum Conditions for Adsorptive Storage
journal, February 2006


The Lennard-Jones equation of state revisited
journal, February 1993


Hydrogen Storage in Carbon Nanostructures: Possibilities and Challenges for Fundamental Molecular Simulations
journal, October 2006


Hydrogen Storage Capacity of Carbon-Foams: Grand Canonical Monte Carlo Simulations
journal, November 2010


Phase equilibrium of quantum fluids from simulation: Hydrogen and neon
journal, May 1997


Molecular Simulation of Adsorption and Diffusion of Hydrogen in Metal−Organic Frameworks
journal, June 2005


Hydrogen Storage in Microporous Metal-Organic Frameworks
journal, May 2003


Understanding Hydrogen Adsorption in Metal−Organic Frameworks with Open Metal Sites:  A Computational Study
journal, January 2006


Covalent Organic Frameworks as Exceptional Hydrogen Storage Materials
journal, September 2008


Experimental and Theoretical Studies of Gas Adsorption in Cu 3 (BTC) 2 :  An Effective Activation Procedure
journal, July 2007


Exceptional H2 Saturation Uptake in Microporous Metal−Organic Frameworks
journal, March 2006


Adsorption of Gases in Metal Organic Materials:  Comparison of Simulations and Experiments
journal, July 2005


Efficient molecular dynamics and hybrid Monte Carlo algorithms for path integrals
journal, August 1993


Merging Porphyrins with Organometallics: Synthesis and Applications
journal, September 2008


Path integral grand canonical Monte Carlo
journal, October 1997


Molecular simulations of adsorption and diffusion of RDX in IRMOF-1
journal, August 2009


Adsorption and Diffusion of Hydrogen in a New Metal−Organic Framework Material:  [Zn(bdc)(ted) 0.5 ]
journal, February 2008


Molecular simulation of hydrogen adsorption in single-walled carbon nanotubes and idealized carbon slit pores
journal, January 1999


Hydrogen Sorption in Functionalized Metal−Organic Frameworks
journal, May 2004

  • Rowsell, Jesse L. C.; Millward, Andrew R.; Park, Kyo Sung
  • Journal of the American Chemical Society, Vol. 126, Issue 18, p. 5666-5667
  • https://doi.org/10.1021/ja049408c

Works referencing / citing this record:

Palladium-catalyzed amination of meso-(bromophenyl)porphyrins with diamines and azamacrocycles
journal, January 2014