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Title: Stress-induced chemical detection using flexible metal-organic frameworks.

Abstract

In this work we demonstrate the concept of stress-induced chemical detection using metal-organic frameworks (MOFs) by integrating a thin film of the MOF HKUST-1 with a microcantilever surface. The results show that the energy of molecular adsorption, which causes slight distortions in the MOF crystal structure, can be efficiently converted to mechanical energy to create a highly responsive, reversible, and selective sensor. This sensor responds to water, methanol, and ethanol vapors, but yields no response to either N{sub 2} or O{sub 2}. The magnitude of the signal, which is measured by a built-in piezoresistor, is correlated with the concentration and can be fitted to a Langmuir isotherm. Furthermore, we show that the hydration state of the MOF layer can be used to impart selectivity to CO{sub 2}. We also report the first use of surface-enhanced Raman spectroscopy to characterize the structure of a MOF film. We conclude that the synthetic versatility of these nanoporous materials holds great promise for creating recognition chemistries to enable selective detection of a wide range of analytes. A force field model is described that successfully predicts changes in MOF properties and the uptake of gases. This model is used to predict adsorption isotherms for amore » number of representative compounds, including explosives, nerve agents, volatile organic compounds, and polyaromatic hydrocarbons. The results show that, as a result of relatively large heats of adsorption (> 20 kcal mol{sup -1}) in most cases, we expect an onset of adsorption by MOF as low as 10{sup -6} kPa, suggesting the potential to detect compounds such as RDX at levels as low as 10 ppb at atmospheric pressure.« less

Authors:
;  [1];  [1];  [1];  [1];  [1]; ;  [2]
+ Show Author Affiliations
  1. (Georgia Institute of Technology, Atlanta, GA)
  2. (National Institute of Standards & Technology, Gaithersburg, MD)
Publication Date:
Research Org.:
Sandia National Laboratories
Sponsoring Org.:
USDOE
OSTI Identifier:
993628
Report Number(s):
SAND2009-6185
TRN: US201024%%96
DOE Contract Number:
AC04-94AL85000
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
10 SYNTHETIC FUELS; 36 MATERIALS SCIENCE; ADSORPTION; ADSORPTION ISOTHERMS; ATMOSPHERIC PRESSURE; CRYSTAL STRUCTURE; DETECTION; ETHANOL; EXPLOSIVES; GASES; HYDRATION; HYDROCARBONS; ISOTHERMS; METHANOL; NERVES; ORGANIC COMPOUNDS; RAMAN SPECTROSCOPY; THIN FILMS; WATER

Citation Formats

Allendorf, Mark D., Hesketh, Peter J., Gall, Kenneth A., Choudhury, A., Pikarsky, J., Andruszkiewicz, Leanne, Houk, Ronald J. T., and Talin, Albert Alec. Stress-induced chemical detection using flexible metal-organic frameworks.. United States: N. p., 2009. Web. doi:10.2172/993628.
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Allendorf, Mark D., Hesketh, Peter J., Gall, Kenneth A., Choudhury, A., Pikarsky, J., Andruszkiewicz, Leanne, Houk, Ronald J. T., & Talin, Albert Alec. Stress-induced chemical detection using flexible metal-organic frameworks.. United States. doi:10.2172/993628.
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Allendorf, Mark D., Hesketh, Peter J., Gall, Kenneth A., Choudhury, A., Pikarsky, J., Andruszkiewicz, Leanne, Houk, Ronald J. T., and Talin, Albert Alec. Tue . "Stress-induced chemical detection using flexible metal-organic frameworks.". United States. doi:10.2172/993628. https://www.osti.gov/servlets/purl/993628.
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@article{osti_993628,
title = {Stress-induced chemical detection using flexible metal-organic frameworks.},
author = {Allendorf, Mark D. and Hesketh, Peter J. and Gall, Kenneth A. and Choudhury, A. and Pikarsky, J. and Andruszkiewicz, Leanne and Houk, Ronald J. T. and Talin, Albert Alec},
abstractNote = {In this work we demonstrate the concept of stress-induced chemical detection using metal-organic frameworks (MOFs) by integrating a thin film of the MOF HKUST-1 with a microcantilever surface. The results show that the energy of molecular adsorption, which causes slight distortions in the MOF crystal structure, can be efficiently converted to mechanical energy to create a highly responsive, reversible, and selective sensor. This sensor responds to water, methanol, and ethanol vapors, but yields no response to either N{sub 2} or O{sub 2}. The magnitude of the signal, which is measured by a built-in piezoresistor, is correlated with the concentration and can be fitted to a Langmuir isotherm. Furthermore, we show that the hydration state of the MOF layer can be used to impart selectivity to CO{sub 2}. We also report the first use of surface-enhanced Raman spectroscopy to characterize the structure of a MOF film. We conclude that the synthetic versatility of these nanoporous materials holds great promise for creating recognition chemistries to enable selective detection of a wide range of analytes. A force field model is described that successfully predicts changes in MOF properties and the uptake of gases. This model is used to predict adsorption isotherms for a number of representative compounds, including explosives, nerve agents, volatile organic compounds, and polyaromatic hydrocarbons. The results show that, as a result of relatively large heats of adsorption (> 20 kcal mol{sup -1}) in most cases, we expect an onset of adsorption by MOF as low as 10{sup -6} kPa, suggesting the potential to detect compounds such as RDX at levels as low as 10 ppb at atmospheric pressure.},
doi = {10.2172/993628},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Sep 01 00:00:00 EDT 2009},
month = {Tue Sep 01 00:00:00 EDT 2009}
}
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DOI:  10.2172/993628
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