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Title: Dense Glass Packing Can Slow Reactions with an Atmospheric Gas

Abstract

Previous work utilizing crystal polymorphs has established the importance of the molecular packing environment for modulating solid–gas reactivity. In our research, we show, for the first time, that the chemical stability of an amorphous material in contact with a reactive gas can be significantly improved by controlling glass packing. Here, we utilize the reaction of indomethacin with ammonia as this system has been well-characterized for crystalline polymorphs. For these experiments, physical vapor deposition (PVD) is used to prepare glasses of indomethacin with a range of densities and thermal stabilities. The indomethacin–ammonia reactivity is assessed through the increase in mass of glassy thin films exposed to ammonia gas, as characterized by a quartz crystal microbalance. Indomethacin glasses vapor-deposited at substrate temperatures below the glass transition temperature (Tg) show unprecedented decrease in reaction rates relative to the liquid-cooled glass, by as much as 1 order of magnitude, with the densest glasses having the slowest reactions. The diminished solubility of ammonia in dense PVD glasses is found to be a major factor in their remarkable chemical stability. As chemically stable amorphous solids are in demand for applications including pharmaceuticals and organic electronics, this work offers a strategy to improve performance of these materials.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1605683
Grant/Contract Number:  
SC0002161
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 123; Journal Issue: 47; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Qiu, Yue, Bieser, Michael E., and Ediger, Mark D.. Dense Glass Packing Can Slow Reactions with an Atmospheric Gas. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.jpcb.9b08360.
Qiu, Yue, Bieser, Michael E., & Ediger, Mark D.. Dense Glass Packing Can Slow Reactions with an Atmospheric Gas. United States. https://doi.org/10.1021/acs.jpcb.9b08360
Qiu, Yue, Bieser, Michael E., and Ediger, Mark D.. Wed . "Dense Glass Packing Can Slow Reactions with an Atmospheric Gas". United States. https://doi.org/10.1021/acs.jpcb.9b08360. https://www.osti.gov/servlets/purl/1605683.
@article{osti_1605683,
title = {Dense Glass Packing Can Slow Reactions with an Atmospheric Gas},
author = {Qiu, Yue and Bieser, Michael E. and Ediger, Mark D.},
abstractNote = {Previous work utilizing crystal polymorphs has established the importance of the molecular packing environment for modulating solid–gas reactivity. In our research, we show, for the first time, that the chemical stability of an amorphous material in contact with a reactive gas can be significantly improved by controlling glass packing. Here, we utilize the reaction of indomethacin with ammonia as this system has been well-characterized for crystalline polymorphs. For these experiments, physical vapor deposition (PVD) is used to prepare glasses of indomethacin with a range of densities and thermal stabilities. The indomethacin–ammonia reactivity is assessed through the increase in mass of glassy thin films exposed to ammonia gas, as characterized by a quartz crystal microbalance. Indomethacin glasses vapor-deposited at substrate temperatures below the glass transition temperature (Tg) show unprecedented decrease in reaction rates relative to the liquid-cooled glass, by as much as 1 order of magnitude, with the densest glasses having the slowest reactions. The diminished solubility of ammonia in dense PVD glasses is found to be a major factor in their remarkable chemical stability. As chemically stable amorphous solids are in demand for applications including pharmaceuticals and organic electronics, this work offers a strategy to improve performance of these materials.},
doi = {10.1021/acs.jpcb.9b08360},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 47,
volume = 123,
place = {United States},
year = {2019},
month = {11}
}

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