Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks
Por favor, use este identificador para citar o enlazar este ítem:
http://hdl.handle.net/10045/108710
Título: | Quest for an Optimal Methane Hydrate Formation in the Pores of Hydrolytically Stable Metal–Organic Frameworks |
---|---|
Autor/es: | Cuadrado-Collados, Carlos | Mouchaham, Georges | Daemen, Luke L. | Cheng, Yongqiang | Ramírez-Cuesta, Anibal J. | Aggarwal, Himanshu | Missyul, Alexander | Eddaoudi, Mohamed | Belmabkhout, Youssef | Silvestre-Albero, Joaquín |
Grupo/s de investigación o GITE: | Materiales Avanzados |
Centro, Departamento o Servicio: | Universidad de Alicante. Departamento de Química Inorgánica | Universidad de Alicante. Instituto Universitario de Materiales |
Palabras clave: | Hydrocarbons | Hydrate formation | Metal organic frameworks | Solvates | Cavities |
Área/s de conocimiento: | Química Inorgánica |
Fecha de publicación: | 11-jul-2020 |
Editor: | American Chemical Society |
Cita bibliográfica: | Journal of the American Chemical Society. 2020, 142(31): 13391-13397. https://doi.org/10.1021/jacs.0c01459 |
Resumen: | Porous metal–organic frameworks (MOFs) capable of storing a relatively high amount of dry methane (CH4) in the adsorbed phase are largely explored; however, solid CH4 storage in confined pores of MOFs in the form of hydrates is yet to be discovered. Here we report a rational approach to form CH4 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 an 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 CH4 storage/delivery process could be drastically reduced compared to the conventional CH4-adsorbed phase storage on the dry Cr-soc-MOF-1 (≤3 MPa vs 10 MPa). |
Patrocinador/es: | G.M., M.E., and Y.B. thank the Aramco sponsored research fund (contract. 66600024505). We would like also to acknowledge the support by King Abdullah University of Science and Technology. J.S.A. would like to acknowledge financial support from the MINECO (MAT2016-80285-p), Generalitat Valenciana (PROMETEOII/2014/004), Oak Ridge beam time availability (Project IPTS-20859.1), and Spanish ALBA synchrotron (Project 2020014008). INS experiments were conducted at the VISION beamline (IPTS-20859) at the Spallation Neutron Source, Oak Ridge National Laboratory (ORNL), which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE), under contract no. DE-AC0500OR22725 with UT Battelle, LLC. The computing resources were made available through the VirtuES and the ICE-MAN projects, funded by the Laboratory Directed Research and Development programme and by Compute and Data Environment for Science (CADES) at ORNL. |
URI: | http://hdl.handle.net/10045/108710 |
ISSN: | 0002-7863 (Print) | 1520-5126 (Online) |
DOI: | 10.1021/jacs.0c01459 |
Idioma: | eng |
Tipo: | info:eu-repo/semantics/article |
Derechos: | © 2020 American Chemical Society |
Revisión científica: | si |
Versión del editor: | https://doi.org/10.1021/jacs.0c01459 |
Aparece en las colecciones: | INV - LMA - Artículos de Revistas |
Archivos en este ítem:
Archivo | Descripción | Tamaño | Formato | |
---|---|---|---|---|
Cuadrado-Collados_etal_2020_JAmChemSoc_final.pdf | Versión final (acceso restringido) | 3,12 MB | Adobe PDF | Abrir Solicitar una copia |
Cuadrado-Collados_etal_2020_JAmChemSoc_accepted.pdf | Accepted Manuscript (acceso abierto) | 718,77 kB | Adobe PDF | Abrir Vista previa |
Todos los documentos en RUA están protegidos por derechos de autor. Algunos derechos reservados.