Critical Factors in Computational Characterization of Hydrogen Storage in Metal–Organic Frameworks

Camp, Jeffrey; Stavila, Vitalie; Allendorf, Mark D.; Prendergast, David; Haranczyk, Maciej

doi:10.1021/acs.jpcc.8b04021

Title: Critical Factors in Computational Characterization of Hydrogen Storage in Metal–Organic Frameworks

Journal Article · Thu Jul 26 00:00:00 EDT 2018 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b04021· OSTI ID:1507406

Camp, Jeffrey ^[1];

^[2];

^[2]; Prendergast, David ^[1];

^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Inconsistencies in high-pressure H2 adsorption data and a lack of comparative experiment–theory studies have made the evaluation of both new and existing metal–organic frameworks (MOFs) challenging in the context of hydrogen storage applications. In this work, we performed grand canonical Monte Carlo (GCMC) simulations in nearly 500 experimentally refined MOF structures to examine the variance in simulation results because of the equation of state, H₂ potential, and the effect of density functional theory structural optimization. We find that hydrogen capacity at 77 K and 100 bar, as well as hydrogen 100-to-5 bar deliverable capacity, is correlated more strongly with the MOF pore volume than with the MOF surface area (the latter correlation is known as the Chahine’s rule). The tested methodologies provide consistent rankings of materials. In addition, four prototypical MOFs (MOF-74, CuBTC, ZIF-8, and MOF-5) with a range of surface areas, pore structures, and surface chemistries, representative of promising adsorbents for hydrogen storage, are evaluated in detail with both GCMC simulations and experimental measurements. Simulations with a three-site classical potential for H₂ agree best with our experimental data except in the case of MOF-5, in which H₂ adsorption is best replicated with a five-site potential. However, for the purpose of ranking materials, these two choices for H₂ potential make little difference. Here more significantly, 100 bar loading estimates based on more accurate equations of state for the vapor–liquid equilibrium yield the best comparisons with the experiment.

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Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1507406

Report Number(s):: SAND-2019-3246J; 673700

Journal Information:: Journal of Physical Chemistry. C, Vol. 122, Issue 33; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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