A Nanocavitation Approach to Understanding Water Capture, Water Release, and Framework Physical Stability in Hierarchically Porous MOFs.

Autor:	Liu J; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States.; School of Chemistry and Materials Science, and Department of Chemical Engineering, Rochester Institute of Technology, Rochester, New York 14623, United States., Prelesnik JL; Department of Chemistry and Chemical Theory Center, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States., Patel R; Department of Chemistry and Chemical Theory Center, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States.; Department of Chemical Engineering and Materials Science, University of Minnesota, 412 Washington Avenue SE, Minneapolis, Minnesota 55455, United States., Kramar BV; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States., Wang R; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States., Malliakas CD; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States., Chen LX; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States.; Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, Illinois 60439, United States., Siepmann JI; Department of Chemistry and Chemical Theory Center, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States.; Department of Chemical Engineering and Materials Science, University of Minnesota, 412 Washington Avenue SE, Minneapolis, Minnesota 55455, United States., Hupp JT; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States.
Jazyk:	angličtina
Zdroj:	Journal of the American Chemical Society [J Am Chem Soc] 2023 Dec 27; Vol. 145 (51), pp. 27975-27983. Date of Electronic Publication: 2023 Dec 12.
DOI:	10.1021/jacs.3c07624
Abstrakt:	Chemically stable metal-organic frameworks (MOFs) featuring interconnected hierarchical pores have proven to be promising for a remarkable variety of applications. Nevertheless, the framework's susceptibility to capillary-force-induced pore collapse, especially during water evacuation, has often limited practical applications. Methodologies capable of predicting the relative magnitudes of these forces as functions of the pore size, chemical composition of the pore walls, and fluid loading would be valuable for resolution of the pore collapse problem. Here, we report that a molecular simulation approach centered on evacuation-induced nanocavitation within fluids occupying MOF pores can yield the desired physical-force information. The computations can spatially pinpoint evacuation elements responsible for collapse and the chemical basis for mitigation of the collapse of modified pores. Experimental isotherms and difference-electron density measurements of the MOF NU-1000 and four chemical variants validate the computational approach and corroborate predictions regarding relative stability, anomalous sequence of pore-filling, and chemical basis for mitigation of destructive forces.
Databáze:	MEDLINE
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