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Title: Anomalous water expulsion from carbon-based rods at high humidity

Abstract

Managing water is critical for industrial applications including CO2 capture, catalysis, bio-oil separations and energy storage. Various classes of materials have been designed for these applications, achieving specific water adsorption capacities at a given relative humidity (RH). Three water adsorption-desorption mechanisms are common to inorganic materials: (1) chemisorption, which may lead to the modification of the first coordination sphere; (2) simple adsorption, which is reversible in nature; or (3) capillary condensation, which is irreversible in nature. Regardless of sorption mechanism, all materials known today increase water adsorption capacity with increasing RH; none exhibit repeated adsorption of water at low humidity and release at high humidity. We present here a material that breaks from this convention: a new class of nitrogen containing carbon rods along with nonstoichiometric FeXSY that adsorb water at low humidity, and spontaneously expel half of the adsorbed water when the RH exceeds a 50–80% threshold. Monolayers of water form on the surfaces of the carbon rods, with the amount of water adsorbed directly linked to the aspect ratio of the rods and the available surface area. This unprecedented water expulsion is a reversible physical process. Once a complete monolayer is formed, adjacent rods in the bundles beginmore » to adhere together via formation of a bridging monolayer, reducing the surface area available for water to adhere to. We believe the unique surface chemistry of these carbon rods can be used on other functionalized materials. Such behaviour offers a paradigm shift in water purification and separation: water could be repeatedly adsorbed from a low humidity vapour stream and then expelled into a pure water vapour stream, or humidity-responsive membranes could change their water permeance or selectivity as a function of RH.« less

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1336003
Report Number(s):
PNNL-SA-112991
Journal ID: ISSN 1748-3387; 48731
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nature Nanotechnology; Journal Volume: 11; Journal Issue: 9
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Nanorods; nanoparticles; nanocomposite; switchable ionic liquids; adsorption; expulsion; Environmental Molecular Sciences Laboratory

Citation Formats

Nune, Satish K., Lao, David B., Heldebrant, David J., Liu, Jian, Olszta, Matthew J., Kukkadapu, Ravi K., Gordon, Lyle M., Nandasiri, Manjula I., Whyatt, Greg, Clayton, Chris, Gotthold, David W., Engelhard, Mark H., and Schaef, Herbert T. Anomalous water expulsion from carbon-based rods at high humidity. United States: N. p., 2016. Web. doi:10.1038/nnano.2016.91.
Nune, Satish K., Lao, David B., Heldebrant, David J., Liu, Jian, Olszta, Matthew J., Kukkadapu, Ravi K., Gordon, Lyle M., Nandasiri, Manjula I., Whyatt, Greg, Clayton, Chris, Gotthold, David W., Engelhard, Mark H., & Schaef, Herbert T. Anomalous water expulsion from carbon-based rods at high humidity. United States. doi:10.1038/nnano.2016.91.
Nune, Satish K., Lao, David B., Heldebrant, David J., Liu, Jian, Olszta, Matthew J., Kukkadapu, Ravi K., Gordon, Lyle M., Nandasiri, Manjula I., Whyatt, Greg, Clayton, Chris, Gotthold, David W., Engelhard, Mark H., and Schaef, Herbert T. Mon . "Anomalous water expulsion from carbon-based rods at high humidity". United States. doi:10.1038/nnano.2016.91.
@article{osti_1336003,
title = {Anomalous water expulsion from carbon-based rods at high humidity},
author = {Nune, Satish K. and Lao, David B. and Heldebrant, David J. and Liu, Jian and Olszta, Matthew J. and Kukkadapu, Ravi K. and Gordon, Lyle M. and Nandasiri, Manjula I. and Whyatt, Greg and Clayton, Chris and Gotthold, David W. and Engelhard, Mark H. and Schaef, Herbert T.},
abstractNote = {Managing water is critical for industrial applications including CO2 capture, catalysis, bio-oil separations and energy storage. Various classes of materials have been designed for these applications, achieving specific water adsorption capacities at a given relative humidity (RH). Three water adsorption-desorption mechanisms are common to inorganic materials: (1) chemisorption, which may lead to the modification of the first coordination sphere; (2) simple adsorption, which is reversible in nature; or (3) capillary condensation, which is irreversible in nature. Regardless of sorption mechanism, all materials known today increase water adsorption capacity with increasing RH; none exhibit repeated adsorption of water at low humidity and release at high humidity. We present here a material that breaks from this convention: a new class of nitrogen containing carbon rods along with nonstoichiometric FeXSY that adsorb water at low humidity, and spontaneously expel half of the adsorbed water when the RH exceeds a 50–80% threshold. Monolayers of water form on the surfaces of the carbon rods, with the amount of water adsorbed directly linked to the aspect ratio of the rods and the available surface area. This unprecedented water expulsion is a reversible physical process. Once a complete monolayer is formed, adjacent rods in the bundles begin to adhere together via formation of a bridging monolayer, reducing the surface area available for water to adhere to. We believe the unique surface chemistry of these carbon rods can be used on other functionalized materials. Such behaviour offers a paradigm shift in water purification and separation: water could be repeatedly adsorbed from a low humidity vapour stream and then expelled into a pure water vapour stream, or humidity-responsive membranes could change their water permeance or selectivity as a function of RH.},
doi = {10.1038/nnano.2016.91},
journal = {Nature Nanotechnology},
number = 9,
volume = 11,
place = {United States},
year = {Mon Jun 13 00:00:00 EDT 2016},
month = {Mon Jun 13 00:00:00 EDT 2016}
}