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Low Temperature Calorimetry Coupled with Molecular Simulations for an In-Depth Characterization of the Guest-Dependent Compliant Behaviour of MOFs

preprint
submitted on 30.01.2020 and posted on 31.01.2020 by Paul Iacomi, Bin Zheng, Simon Krause, Stefan Kaskel, Guillaume Maurin, Philip L. Llewellyn
In this study adsorption microcalorimetry is employed to monitor the adsorption of four probes (argon, oxygen, nitrogen and carbon monoxide) on a highly flexible mesoporous metal-organic framework (DUT-49, DUT = Dresden University of Technology), precisely measuring the differential enthalpy of adsorption alongside high-resolution isotherms. This experimental approach combined with force field Monte Carlo simulations reveals distinct pore filling adsorption behaviours for the selected probes, with argon and oxygen showing abrupt adsorption in the open pore form of DUT-49, in contrast with the gradual filling for nitrogen and carbon monoxide. A complex structural transition behaviour of DUT-49 observed upon nitrogen adsorption is elucidated through an isotherm deconvolution in order to quantify the fraction of the open pore, contracted pore and intermediate pore forms that coexists at a given gas pressure. Finally, the heat flow measured during the guest-induced structural contraction of DUT-49 allowed an exploration of complex open-contracted pore transition energetics, leading to a first assessment of the energy required to induce this spectacular structural change.

Funding

DEFect NETwork materials science and engineering

European Commission

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Mechanical Control of Pore Architecture to intelligently modulate molecular capture/separation/regeneration – MeaCoPA

Agence Nationale de la Recherche

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Fundamental Understanding of Negative Gas Adsorption in Mesoporous Solids: Towards threshold sensitive mechanical actuators

Deutsche Forschungsgemeinschaft

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Fundamental Understanding of Negative Gas Adsorption in Mesoporous Solids: Towards threshold sensitive mechanical actuators – FUN

Agence Nationale de la Recherche

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History

Email Address of Submitting Author

mail@pauliacomi.com

Institution

Institut Charles Gerhardt Montpellier

Country

France

ORCID For Submitting Author

0000-0001-5477-1503

Declaration of Conflict of Interest

No conflict of interest to declare

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