Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches

11 pags., 9 figs.

Bibliographic Details
Authors: Cabrera-Ramírez, Adriana, Arismendi-Arrieta, D.J., Valdés, Álvaro, Prosmiti, Rita
Format: article
Status:Versión aceptada para publicación
Publication Date:2020
Country:España
Institution:Consejo Superior de Investigaciones Científicas (CSIC)
Repository:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/233433
Online Access:http://hdl.handle.net/10261/233433
Access Level:Open access
Keyword:CO2clathrate hydrates
CO2storage
Electronicstructure calculations
Guest-host interactions
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spelling Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional ApproachesCabrera-Ramírez, AdrianaArismendi-Arrieta, D.J.Valdés, ÁlvaroProsmiti, RitaCO2clathrate hydratesCO2storageElectronicstructure calculationsGuest-host interactions11 pags., 9 figs.The formation of specific clathrate hydrates and their trans-formation at given thermodynamic conditions depends on theinteractions between the guest molecule/s and the host waterlattice. Understanding their structural stability is essential tocontrol structure-property relations involved in different tech-nological applications. Thus, the energetic aspects relative toCO2@sI clathrate hydrate are investigated through the compu-tation of the underlying interactions, dominated by hydrogenbonds and van der Waals forces, from first-principles electronicstructure approaches. The stability of the CO2@sI clathrate isevaluated by combining bottom-up and top-down approaches.Guest-free and CO2guest-filled aperiodic cages, up to thegradually CO2occupation of the entire sI periodic unit cellswere considered. Saturation, cohesive and binding energies forthe systems are determined by employing a variety of densityfunctionals and their performance is assessed. The dispersioncorrections on the non-covalent interactions are found to beimportant in the stabilization of the CO2@sI energies, with theencapsulation of the CO2into guest-free/empty cage/latticebeing always an energetically favorable process for most of thefunctionals studied. The PW86PBE functional with XDM orD3(BJ) dispersion corrections predicts a lattice constant inaccord to the experimental values available, and simultaneouslyprovides a reliable description for the guest-host interactions inthe periodic CO2@sI crystal, as well as the energetics of itsprogressive single cage occupancy process. It has been foundthat the preferential orientation of the single CO2in the large sIcrystal cages has a stabilizing effect on the hydrate, concludingthat the CO2@sI structure is favored either by considering theindividual building block cages or the complete sI unit cellcrystal. Such benchmark and methodology cross-check studiesbenefit new data-driven model research by providing high-quality training information, with new insights that indicate theunderlying factors governing their structure-driven stability,and triggering further investigations for controlling the stabili-zation of these promising long-term CO2storage materials.The authors acknowledge the “Centro de Calculo del IFF/SGAI”(CSIC) and CESGA-Supercomputingg centre for allocation ofcomputer time. This work has been supported by MINECO grantNo. FIS2017-83157-P, Comunidad de Madrid grant No. IND2017-AMB7696, “CSIC for Development“ (i-COOP) grant ref:ICOOPB20214, Hermes code:49572 (Universidad Nacional de Colombia) and COST Action CA18212(MD-GAS).Peer reviewedJohn Wiley & SonsCSIC - Instituto de Física Fundamental (IFF)Centro de Supercomputación de GaliciaMinisterio de Economía y Competitividad (España)Comunidad de MadridUniversidad Nacional de ColombiaConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202120212020info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/233433reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/FIS2017-83157-Phttp://doi.org/10.1002/cphc.202001035Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2334332026-05-22T06:33:51Z
dc.title.none.fl_str_mv Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
title Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
spellingShingle Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
Cabrera-Ramírez, Adriana
CO2clathrate hydrates
CO2storage
Electronicstructure calculations
Guest-host interactions
title_short Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
title_full Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
title_fullStr Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
title_full_unstemmed Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
title_sort Exploring CO2@sI Clathrate Hydrates as CO2Storage Agentsby Computational Density Functional Approaches
dc.creator.none.fl_str_mv Cabrera-Ramírez, Adriana
Arismendi-Arrieta, D.J.
Valdés, Álvaro
Prosmiti, Rita
author Cabrera-Ramírez, Adriana
author_facet Cabrera-Ramírez, Adriana
Arismendi-Arrieta, D.J.
Valdés, Álvaro
Prosmiti, Rita
author_role author
author2 Arismendi-Arrieta, D.J.
Valdés, Álvaro
Prosmiti, Rita
author2_role author
author
author
dc.contributor.none.fl_str_mv CSIC - Instituto de Física Fundamental (IFF)
Centro de Supercomputación de Galicia
Ministerio de Economía y Competitividad (España)
Comunidad de Madrid
Universidad Nacional de Colombia
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv CO2clathrate hydrates
CO2storage
Electronicstructure calculations
Guest-host interactions
topic CO2clathrate hydrates
CO2storage
Electronicstructure calculations
Guest-host interactions
description 11 pags., 9 figs.
publishDate 2020
dc.date.none.fl_str_mv 2020
2021
2021
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/233433
url http://hdl.handle.net/10261/233433
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/FIS2017-83157-P
http://doi.org/10.1002/cphc.202001035
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv John Wiley & Sons
publisher.none.fl_str_mv John Wiley & Sons
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869403223193812992
score 15,812429

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