HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation
The development of nanostructured composites made of metal-organic frameworks (MOFs) and graphene-based components, including exfoliated nanoplates of graphene oxide (GO) or reduced (rGO) graphene oxide, is an area of great interest in gas storage and separation. To improve the industrial viability,...
| Autores: | , , , , , , , , , |
|---|---|
| Formato: | artículo |
| Estado: | Versión aceptada para publicación |
| Fecha de publicación: | 2021 |
| País: | España |
| Recursos: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositorio: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/261185 |
| Acesso em linha: | http://hdl.handle.net/10261/261185 https://api.elsevier.com/content/abstract/scopus_id/85119131002 |
| Access Level: | acceso abierto |
| Palavra-chave: | aerogels composite materials gas adsorption Gas separation HKUST-1/GO supercritical CO2 |
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| dc.title.none.fl_str_mv |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| title |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| spellingShingle |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation Rosado, Albert aerogels composite materials gas adsorption Gas separation HKUST-1/GO supercritical CO2 |
| title_short |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| title_full |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| title_fullStr |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| title_full_unstemmed |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| title_sort |
HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and Separation |
| dc.creator.none.fl_str_mv |
Rosado, Albert Borrás, Alejandro Fraile, Julio Navarro, Jorge A.R. Suárez García, Fabián Stylianou, Kyriakos C. López Periago, Ana M. Giner Planas, José Domingo, Concepción Yazdi, Amirali |
| author |
Rosado, Albert |
| author_facet |
Rosado, Albert Borrás, Alejandro Fraile, Julio Navarro, Jorge A.R. Suárez García, Fabián Stylianou, Kyriakos C. López Periago, Ana M. Giner Planas, José Domingo, Concepción Yazdi, Amirali |
| author_role |
author |
| author2 |
Borrás, Alejandro Fraile, Julio Navarro, Jorge A.R. Suárez García, Fabián Stylianou, Kyriakos C. López Periago, Ana M. Giner Planas, José Domingo, Concepción Yazdi, Amirali |
| author2_role |
author author author author author author author author author |
| dc.contributor.none.fl_str_mv |
Ministerio de Ciencia e Innovación (España) Rosado, Albert [0000-0003-3222-9566] Fraile, Julio [0000-0003-2961-7920] Navarro, Jorge A.R. [0000-0002-8359-0397] Stylianou, Kyriakos C.[0000-0003-1670-0020] Suárez García, Fabián [0000-0002-1970-293X] López Periago, Ana M. [0000-0002-3777-3205] Planas, José Giner [0000-0002-1648-2169] Domingo, Concepción [0000-0002-6976-8283] Yazdi, Amirali [0000-0001-9420-8504] Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72] |
| dc.subject.none.fl_str_mv |
aerogels composite materials gas adsorption Gas separation HKUST-1/GO supercritical CO2 |
| topic |
aerogels composite materials gas adsorption Gas separation HKUST-1/GO supercritical CO2 |
| description |
The development of nanostructured composites made of metal-organic frameworks (MOFs) and graphene-based components, including exfoliated nanoplates of graphene oxide (GO) or reduced (rGO) graphene oxide, is an area of great interest in gas storage and separation. To improve the industrial viability, it is commonly demanded to build these nanocomposites with the shape of compact units, such as monoliths, foams, pellets, or films. Methods to generate those 3D nanocomposites involving rGO are abundant; however, they become scarce when GO is the desired support due to the difficulty in maintaining the carbon matrix oxidized during the structuration process. In this work, a methodology based on the use of supercritical CO2 (scCO2) is described for the synthesis of nanocomposites involving a discontinuous MOF phase, e.g. nanoparticles (NPs) of HKUST-1, decorating the surface of a continuous GO matrix, with surface oxygen groups favoring MOF attachment. The use of this new supercritical methodology allows the nanostructuration of the composite in the form of 3D aerogels while avoiding the reduction of GO. Enhanced values of textural properties, determined by low-temperature N2 adsorption-desorption, were observed for the nanocomposites in comparison to the values calculated for similar physical mixtures, highlighting an increase of 40-45% in the value of the surface area for samples with a high percentage of HKUST-1. Moreover, the composite aerogels, displaying a type II isotherm, outperform pristine HKUST-1 in regard to the CH4 practical working capacity at high pressure. Particularly, a composite exhibiting more than 2-fold the working capacity of net HKUST-1 NPs was obtained. Columns involving the composite aerogel as the stationary phase were used to study the separation of N2/CO2 and CH4/CO2 gas mixtures. The results showed a high selectivity of the nanostructured HKUST-1@GO composites for CO2, with breakthrough times of ca. 20 min g-1 and stable cyclic operations. |
| publishDate |
2021 |
| dc.date.none.fl_str_mv |
2021 2022 2022 |
| 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/10261/261185 https://api.elsevier.com/content/abstract/scopus_id/85119131002 |
| url |
http://hdl.handle.net/10261/261185 https://api.elsevier.com/content/abstract/scopus_id/85119131002 |
| dc.language.none.fl_str_mv |
Inglés |
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Inglés |
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info:eu-repo/semantics/openAccess |
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openAccess |
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American Chemical Society |
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American Chemical Society |
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reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC instname:Consejo Superior de Investigaciones Científicas (CSIC) |
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Consejo Superior de Investigaciones Científicas (CSIC) |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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HKUST-1 Metal–Organic Framework Nanoparticle/Graphene Oxide Nanocomposite Aerogels for CO2 and CH4 Adsorption and SeparationRosado, AlbertBorrás, AlejandroFraile, JulioNavarro, Jorge A.R.Suárez García, FabiánStylianou, Kyriakos C.López Periago, Ana M.Giner Planas, JoséDomingo, ConcepciónYazdi, Amiraliaerogelscomposite materialsgas adsorptionGas separationHKUST-1/GOsupercritical CO2The development of nanostructured composites made of metal-organic frameworks (MOFs) and graphene-based components, including exfoliated nanoplates of graphene oxide (GO) or reduced (rGO) graphene oxide, is an area of great interest in gas storage and separation. To improve the industrial viability, it is commonly demanded to build these nanocomposites with the shape of compact units, such as monoliths, foams, pellets, or films. Methods to generate those 3D nanocomposites involving rGO are abundant; however, they become scarce when GO is the desired support due to the difficulty in maintaining the carbon matrix oxidized during the structuration process. In this work, a methodology based on the use of supercritical CO2 (scCO2) is described for the synthesis of nanocomposites involving a discontinuous MOF phase, e.g. nanoparticles (NPs) of HKUST-1, decorating the surface of a continuous GO matrix, with surface oxygen groups favoring MOF attachment. The use of this new supercritical methodology allows the nanostructuration of the composite in the form of 3D aerogels while avoiding the reduction of GO. Enhanced values of textural properties, determined by low-temperature N2 adsorption-desorption, were observed for the nanocomposites in comparison to the values calculated for similar physical mixtures, highlighting an increase of 40-45% in the value of the surface area for samples with a high percentage of HKUST-1. Moreover, the composite aerogels, displaying a type II isotherm, outperform pristine HKUST-1 in regard to the CH4 practical working capacity at high pressure. Particularly, a composite exhibiting more than 2-fold the working capacity of net HKUST-1 NPs was obtained. Columns involving the composite aerogel as the stationary phase were used to study the separation of N2/CO2 and CH4/CO2 gas mixtures. The results showed a high selectivity of the nanostructured HKUST-1@GO composites for CO2, with breakthrough times of ca. 20 min g-1 and stable cyclic operations.This work was supported by the Spanish Ministry of Science and Innovation MICINN through the Severo Ochoa Program for Centers of Excellence (SEV-2015-0496 and CEX2019-000917-S) and the Spanish National Plan of Research with projects CTQ2017-83632, PID2020-115631GB-I00, CTQ2016-75150-R, CTQ2017-84692-R, RTI2018-100832-B-I00, and PID2019-106832RB-I00. J.A.R.N. thanks Junta de Andalucia (P18-RT-612). K.C.S. thanks the Department of Chemistry through start-up funding. This work has been done in the framework of the doctoral program “Chemistry” of the Universitat Autònoma de Barcelona by A.R., A.B., and J.F.; A.R. and A.B. acknowledge FPI grants.Peer reviewedAmerican Chemical SocietyMinisterio de Ciencia e Innovación (España)Rosado, Albert [0000-0003-3222-9566]Fraile, Julio [0000-0003-2961-7920]Navarro, Jorge A.R. [0000-0002-8359-0397]Stylianou, Kyriakos C.[0000-0003-1670-0020]Suárez García, Fabián [0000-0002-1970-293X]López Periago, Ana M. [0000-0002-3777-3205]Planas, José Giner [0000-0002-1648-2169]Domingo, Concepción [0000-0002-6976-8283]Yazdi, Amirali [0000-0001-9420-8504]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202220222021info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/261185https://api.elsevier.com/content/abstract/scopus_id/85119131002reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2017-83632-C2-1-Pinfo:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2016-75150-Rinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2017-84692-Rinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-100832-B-I00info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-106832RB-I00ACS Applied Nano Materialshttps://doi.org/10.1021/acsanm.1c03301Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2611852026-05-22T06:33:51Z |
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15,812429 |