Local structure and distortions of mixed methane-carbon dioxide hydrates

Abstract A vast source of methane is found in gas hydrate deposits, which form naturally dispersed throughout ocean sediments and arctic permafrost. Methane may be obtained from hydrates by exchange with hydrocarbon byproduct carbon dioxide. It is imperative for the development of safe methane extra...

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Published in:Communications Chemistry
Main Authors: Cladek, Bernadette R., Everett, S. Michelle, McDonnell, Marshall T., Tucker, Matthew G., Keffer, David J., Rawn, Claudia J.
Format: Article in Journal/Newspaper
Language:English
Published: Springer Science and Business Media LLC 2021
Subjects:
Online Access:http://dx.doi.org/10.1038/s42004-020-00441-7
http://www.nature.com/articles/s42004-020-00441-7.pdf
http://www.nature.com/articles/s42004-020-00441-7
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spelling crspringernat:10.1038/s42004-020-00441-7 2023-05-15T15:04:48+02:00 Local structure and distortions of mixed methane-carbon dioxide hydrates Cladek, Bernadette R. Everett, S. Michelle McDonnell, Marshall T. Tucker, Matthew G. Keffer, David J. Rawn, Claudia J. 2021 http://dx.doi.org/10.1038/s42004-020-00441-7 http://www.nature.com/articles/s42004-020-00441-7.pdf http://www.nature.com/articles/s42004-020-00441-7 en eng Springer Science and Business Media LLC https://creativecommons.org/licenses/by/4.0 https://creativecommons.org/licenses/by/4.0 CC-BY Communications Chemistry volume 4, issue 1 ISSN 2399-3669 Materials Chemistry Biochemistry Environmental Chemistry General Chemistry journal-article 2021 crspringernat https://doi.org/10.1038/s42004-020-00441-7 2022-01-04T10:04:21Z Abstract A vast source of methane is found in gas hydrate deposits, which form naturally dispersed throughout ocean sediments and arctic permafrost. Methane may be obtained from hydrates by exchange with hydrocarbon byproduct carbon dioxide. It is imperative for the development of safe methane extraction and carbon dioxide sequestration to understand how methane and carbon dioxide co-occupy the same hydrate structure. Pair distribution functions (PDFs) provide atomic-scale structural insight into intermolecular interactions in methane and carbon dioxide hydrates. We present experimental neutron PDFs of methane, carbon dioxide and mixed methane-carbon dioxide hydrates at 10 K analyzed with complementing classical molecular dynamics simulations and Reverse Monte Carlo fitting. Mixed hydrate, which forms during the exchange process, is more locally disordered than methane or carbon dioxide hydrates. The behavior of mixed gas species cannot be interpolated from properties of pure compounds, and PDF measurements provide important understanding of how the guest composition impacts overall order in the hydrate structure. Article in Journal/Newspaper Arctic permafrost Springer Nature (via Crossref) Arctic Communications Chemistry 4 1
institution Open Polar
collection Springer Nature (via Crossref)
op_collection_id crspringernat
language English
topic Materials Chemistry
Biochemistry
Environmental Chemistry
General Chemistry
spellingShingle Materials Chemistry
Biochemistry
Environmental Chemistry
General Chemistry
Cladek, Bernadette R.
Everett, S. Michelle
McDonnell, Marshall T.
Tucker, Matthew G.
Keffer, David J.
Rawn, Claudia J.
Local structure and distortions of mixed methane-carbon dioxide hydrates
topic_facet Materials Chemistry
Biochemistry
Environmental Chemistry
General Chemistry
description Abstract A vast source of methane is found in gas hydrate deposits, which form naturally dispersed throughout ocean sediments and arctic permafrost. Methane may be obtained from hydrates by exchange with hydrocarbon byproduct carbon dioxide. It is imperative for the development of safe methane extraction and carbon dioxide sequestration to understand how methane and carbon dioxide co-occupy the same hydrate structure. Pair distribution functions (PDFs) provide atomic-scale structural insight into intermolecular interactions in methane and carbon dioxide hydrates. We present experimental neutron PDFs of methane, carbon dioxide and mixed methane-carbon dioxide hydrates at 10 K analyzed with complementing classical molecular dynamics simulations and Reverse Monte Carlo fitting. Mixed hydrate, which forms during the exchange process, is more locally disordered than methane or carbon dioxide hydrates. The behavior of mixed gas species cannot be interpolated from properties of pure compounds, and PDF measurements provide important understanding of how the guest composition impacts overall order in the hydrate structure.
format Article in Journal/Newspaper
author Cladek, Bernadette R.
Everett, S. Michelle
McDonnell, Marshall T.
Tucker, Matthew G.
Keffer, David J.
Rawn, Claudia J.
author_facet Cladek, Bernadette R.
Everett, S. Michelle
McDonnell, Marshall T.
Tucker, Matthew G.
Keffer, David J.
Rawn, Claudia J.
author_sort Cladek, Bernadette R.
title Local structure and distortions of mixed methane-carbon dioxide hydrates
title_short Local structure and distortions of mixed methane-carbon dioxide hydrates
title_full Local structure and distortions of mixed methane-carbon dioxide hydrates
title_fullStr Local structure and distortions of mixed methane-carbon dioxide hydrates
title_full_unstemmed Local structure and distortions of mixed methane-carbon dioxide hydrates
title_sort local structure and distortions of mixed methane-carbon dioxide hydrates
publisher Springer Science and Business Media LLC
publishDate 2021
url http://dx.doi.org/10.1038/s42004-020-00441-7
http://www.nature.com/articles/s42004-020-00441-7.pdf
http://www.nature.com/articles/s42004-020-00441-7
geographic Arctic
geographic_facet Arctic
genre Arctic
permafrost
genre_facet Arctic
permafrost
op_source Communications Chemistry
volume 4, issue 1
ISSN 2399-3669
op_rights https://creativecommons.org/licenses/by/4.0
https://creativecommons.org/licenses/by/4.0
op_rightsnorm CC-BY
op_doi https://doi.org/10.1038/s42004-020-00441-7
container_title Communications Chemistry
container_volume 4
container_issue 1
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