Mild-Temperature Supercritical Water Confined in Hydrophobic Metal–Organic Frameworks

Merchiori, Sebastiano; Le Donne, Andrea; Littlefair, Josh D.; Lowe, Alexander Rowland; Yu, Jiang-Jing; Wu, Xu-Dong; Li, Mian; Li, Dan; Geppert-Rybczyńska, Monika; Scheller, Lukasz; Trump, Benjamin A.; Yakovenko, Andrey A.; Zajdel, Paweł; Chorążewski, Mirosław; Grosu, Yaroslav; Meloni, Simone

doi:10.1021/jacs.4c01226

Title: Mild-Temperature Supercritical Water Confined in Hydrophobic Metal–Organic Frameworks

Journal Article · 03 May 2024 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.4c01226 · OSTI ID:2469966

^[1];

^[1]; Littlefair, Josh D. ^[1];

^[2]; Yu, Jiang-Jing ^[3];

^[3];

^[4];

^[2];

^[5]; Trump, Benjamin A. ^[6]; Yakovenko, Andrey A. ^[7];

^[5];

^[8];

^[9];

^[1]

University of Ferrara (Italy)
University of Silesia, Katowice (Poland)
Shantou University, Guangdong (China)
Jinan University, Guangzhou (China)
University of Silesia, Chorzów (Poland)
National Institute of Standards and Technology, Gaithersburg, MD (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
University of Silesia, Katowice,(Poland)
University of Silesia, Katowice (Poland); Basque Research and Technology Alliance (BRTA), Vitoria-Gasteiz (Spain)

Fluids under extreme confinement show characteristics significantly different from those of their bulk counterpart. This work focuses on water confined within the complex cavities of highly hydrophobic metal–organic frameworks (MOFs) at high pressures. A combination of high-pressure intrusion–extrusion experiments with molecular dynamic simulations and synchrotron data reveals that supercritical transition for MOF-confined water takes place at a much lower temperature than in bulk water, ~250 K below the reference values. This large shifting of the critical temperature (T_c) is attributed to the very large density of confined water vapor in the peculiar geometry and chemistry of the cavities of Cu₂tebpz (tebpz = 3,3',5,5'-tetraethyl-4,4'-bipyrazolate) hydrophobic MOF. This is the first time the shift of Tc is investigated for water confined within highly hydrophobic nanoporous materials, which explains why such a large reduction of the critical temperature was never reported before, neither experimentally nor computationally.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China; Guangdong Basic and Applied Basic Research Foundation

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2469966

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 19 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry
Critical constants
Hydrophobicity
Liquids
Metal organic frameworks
Water

Title: Mild-Temperature Supercritical Water Confined in Hydrophobic Metal–Organic Frameworks

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