Hydrogen bonding structure of confined water templated by a metal-organic framework with open metal sites
Name
s41467-019-12751-z.pdf
Description
Published version
Size
2.12 MB
Format
Adobe PDF
Checksum (MD5)
9ef5f0009d9202f5178791e46b763196
Author(s)
Rieth, Adam Joseph
Dinca, Mircea
Date Issued
October 2019
Journal
Nature Communications
Publisher
Springer Science and Business Media LLC
Citation
Rieth, Adam J. et al. “Hydrogen bonding structure of confined water templated by a metal-organic framework with open metal sites.” Nature Communications, vol. 10, 2019, 4771 © 2019 The Author(s)
Version
Final published version
Abstract
Water in confinement exhibits properties significantly different from bulk water due to frustration in the hydrogen-bond network induced by interactions with the substrate. Here, we combine infrared spectroscopy and many-body molecular dynamics simulations to probe the structure and dynamics of confined water as a function of relative humidity within a metal-organic framework containing cylindrical pores lined with ordered cobalt open coordination sites. Building upon the agreement between experimental and theoretical spectra, we demonstrate that water at low relative humidity binds initially to open metal sites and subsequently forms disconnected one-dimensional chains of hydrogen-bonded water molecules bridging between cobalt atoms. With increasing relative humidity, these water chains nucleate pore filling, and water molecules occupy the entire pore interior before the relative humidity reaches 30%. Systematic analysis of rotational and translational dynamics indicates heterogeneity in this pore-confined water, with water molecules displaying variable mobility as a function of distance from the interface.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
Creative Commons Attribution 4.0 International license
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1038/s41467-019-12751-z
