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Unraveling the Water Adsorption Mechanism in the Mesoporous MIL-100(Fe) Metal–Organic Framework
journal contribution
posted on 2019-09-11, 14:45 authored by Paulo
G. M. Mileo, Kyung Ho Cho, Jaedeuk Park, Sabine Devautour-Vinot, Jong-San Chang, Guillaume MaurinAdsorption-based
heat transfer (AHT) devices are promising alternatives
for green energy production and (re)usage; however, they are still
limited by the low performance of their benchmark adsorbent materials.
Metal–organic frameworks (MOFs) have been ranked among the
most promising water adsorbents for this application owing to their
potential superior water uptake and moderate hydrophilicity. However,
there is still a need to rationalize and understand at the microscopic
scale the water adsorption performances of this family of materials
to further guide the selection of the next-generation water adsorbents.
In this context, a full understanding of the water adsorption mechanism
in the most promising MOFs containing coordinated unsaturated sites
is still highly challenging. Here, we explore the water adsorption
in the mesoporous MOF MIL-100(Fe) containing coordinated unsaturated
Fe(III) sites by combining advanced modeling and experimental tools.
As a first stage, density functional theory calculations are performed
to derive an accurate force field to describe the specific interactions
between water and the coordinated unsaturated Fe(III) sites. This
force field is further implemented in a grand canonical Monte Carlo
scheme to simulate the water adsorption isotherm and enthalpy in the
whole range of relative pressures. A validation of the microscopic
models and force field parameters is gained from a very good agreement
between the experimental and simulated water adsorption data. As a
further step, we provide an unprecedented description of the water
adsorption microscopic mechanism in this very promising AHT water
adsorbent by a careful analysis of the MIL-100(Fe)/H2O
interactions at low and intermediate relative pressures as well as
the hydrogen bond network and cluster formation at higher relative
pressure.
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MILAHT water adsorbentbenchmark adsorbent materialsforce fieldMOFforce field parameterswater adsorption performanceswater adsorption datanext-generation water adsorbentshydrogen bond networkcanonical Monte Carlo schemewater adsorption mechanismwater adsorption isothermWater Adsorption Mechanismwater adsorption
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