Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks
International audience Porous MOFs capable of storing relatively high amount of dry methane (CH 4) in adsorbed phase are largely explored, however solid CH 4 storage in confined pores of MOFs in the form of hydrates is yet to be discovered. Here we report a rational approach to form CH 4 hydrates by...
Published in: | Journal of the American Chemical Society |
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Online Access: | https://hal.archives-ouvertes.fr/hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519/document https://hal.archives-ouvertes.fr/hal-03090519/file/2020_JACS_Preprint.pdf https://doi.org/10.1021/jacs.0c01459 |
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ftunivnantes:oai:HAL:hal-03090519v1 2023-05-15T17:11:51+02:00 Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks Cuadrado-Collados, Carlos Mouchaham, Georges Daemen, Luke Cheng, Yongqiang Ramirez-Cuesta, Anibal Aggarwal, Himanshu Missyul, Alexander Eddaoudi, Mohamed Belmabkhout, Youssef Silvestre-Albero, Joaquin Universidad de Alicante King Abdullah University of Science and Technology (KAUST) Oak Ridge National Laboratory Oak Ridge (ORNL) UT-Battelle, LLC Spallation Neutron Source UT-Battelle, LLC-UT-Battelle, LLC Thermodynamics FPMS 2020-08-05 https://hal.archives-ouvertes.fr/hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519/document https://hal.archives-ouvertes.fr/hal-03090519/file/2020_JACS_Preprint.pdf https://doi.org/10.1021/jacs.0c01459 en eng HAL CCSD American Chemical Society info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.0c01459 hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519/document https://hal.archives-ouvertes.fr/hal-03090519/file/2020_JACS_Preprint.pdf doi:10.1021/jacs.0c01459 info:eu-repo/semantics/OpenAccess ISSN: 0002-7863 EISSN: 1520-5126 Journal of the American Chemical Society https://hal.archives-ouvertes.fr/hal-03090519 Journal of the American Chemical Society, American Chemical Society, 2020, 142 (31), pp.13391-13397. ⟨10.1021/jacs.0c01459⟩ [CHIM]Chemical Sciences info:eu-repo/semantics/article Journal articles 2020 ftunivnantes https://doi.org/10.1021/jacs.0c01459 2022-09-13T23:09:34Z International audience Porous MOFs capable of storing relatively high amount of dry methane (CH 4) in adsorbed phase are largely explored, however solid CH 4 storage in confined pores of MOFs in the form of hydrates is yet to be discovered. Here we report a rational approach to form CH 4 hydrates by taking advantage of the optimal pore confinement in relatively narrow cavities of hydrolytically stable MOFs. Unprecedentedly, we were able to isolate methane hydrate (MH) nanocrystals with a sI structure encapsulated inside MOF pores with an optimal cavity dimension. It was found, that confined nanocrystals require cavities slightly larger than the unit cell crystal size of MHs (1.2 nm), as exemplified in the experimental case study performed on Cr-soc-MOF-1 vs smaller cavities of Y-shp-MOF-5. Under these conditions, the excess amount of methane stored in the pores of Cr-soc-MOF-1 in the form of MH was found to be ≈50% larger than the corresponding dry adsorbed amount at 10 MPa. More importantly, the pressure gradient driving the CH 4 storage/delivery process could be drastically reduced compared to the conventional CH 4 adsorbed phase storage on the dry Cr-soc-MOF-1 (≤3 MPa vs. 10 MPa) Article in Journal/Newspaper Methane hydrate Université de Nantes: HAL-UNIV-NANTES Journal of the American Chemical Society 142 31 13391 13397 |
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Université de Nantes: HAL-UNIV-NANTES |
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ftunivnantes |
language |
English |
topic |
[CHIM]Chemical Sciences |
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[CHIM]Chemical Sciences Cuadrado-Collados, Carlos Mouchaham, Georges Daemen, Luke Cheng, Yongqiang Ramirez-Cuesta, Anibal Aggarwal, Himanshu Missyul, Alexander Eddaoudi, Mohamed Belmabkhout, Youssef Silvestre-Albero, Joaquin Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
topic_facet |
[CHIM]Chemical Sciences |
description |
International audience Porous MOFs capable of storing relatively high amount of dry methane (CH 4) in adsorbed phase are largely explored, however solid CH 4 storage in confined pores of MOFs in the form of hydrates is yet to be discovered. Here we report a rational approach to form CH 4 hydrates by taking advantage of the optimal pore confinement in relatively narrow cavities of hydrolytically stable MOFs. Unprecedentedly, we were able to isolate methane hydrate (MH) nanocrystals with a sI structure encapsulated inside MOF pores with an optimal cavity dimension. It was found, that confined nanocrystals require cavities slightly larger than the unit cell crystal size of MHs (1.2 nm), as exemplified in the experimental case study performed on Cr-soc-MOF-1 vs smaller cavities of Y-shp-MOF-5. Under these conditions, the excess amount of methane stored in the pores of Cr-soc-MOF-1 in the form of MH was found to be ≈50% larger than the corresponding dry adsorbed amount at 10 MPa. More importantly, the pressure gradient driving the CH 4 storage/delivery process could be drastically reduced compared to the conventional CH 4 adsorbed phase storage on the dry Cr-soc-MOF-1 (≤3 MPa vs. 10 MPa) |
author2 |
Universidad de Alicante King Abdullah University of Science and Technology (KAUST) Oak Ridge National Laboratory Oak Ridge (ORNL) UT-Battelle, LLC Spallation Neutron Source UT-Battelle, LLC-UT-Battelle, LLC Thermodynamics FPMS |
format |
Article in Journal/Newspaper |
author |
Cuadrado-Collados, Carlos Mouchaham, Georges Daemen, Luke Cheng, Yongqiang Ramirez-Cuesta, Anibal Aggarwal, Himanshu Missyul, Alexander Eddaoudi, Mohamed Belmabkhout, Youssef Silvestre-Albero, Joaquin |
author_facet |
Cuadrado-Collados, Carlos Mouchaham, Georges Daemen, Luke Cheng, Yongqiang Ramirez-Cuesta, Anibal Aggarwal, Himanshu Missyul, Alexander Eddaoudi, Mohamed Belmabkhout, Youssef Silvestre-Albero, Joaquin |
author_sort |
Cuadrado-Collados, Carlos |
title |
Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
title_short |
Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
title_full |
Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
title_fullStr |
Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
title_full_unstemmed |
Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
title_sort |
quest for an optimal methane hydrate formation in the pores of hydrolytically stable metal–organic frameworks |
publisher |
HAL CCSD |
publishDate |
2020 |
url |
https://hal.archives-ouvertes.fr/hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519/document https://hal.archives-ouvertes.fr/hal-03090519/file/2020_JACS_Preprint.pdf https://doi.org/10.1021/jacs.0c01459 |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
ISSN: 0002-7863 EISSN: 1520-5126 Journal of the American Chemical Society https://hal.archives-ouvertes.fr/hal-03090519 Journal of the American Chemical Society, American Chemical Society, 2020, 142 (31), pp.13391-13397. ⟨10.1021/jacs.0c01459⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.0c01459 hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519 https://hal.archives-ouvertes.fr/hal-03090519/document https://hal.archives-ouvertes.fr/hal-03090519/file/2020_JACS_Preprint.pdf doi:10.1021/jacs.0c01459 |
op_rights |
info:eu-repo/semantics/OpenAccess |
op_doi |
https://doi.org/10.1021/jacs.0c01459 |
container_title |
Journal of the American Chemical Society |
container_volume |
142 |
container_issue |
31 |
container_start_page |
13391 |
op_container_end_page |
13397 |
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1766068601122455552 |