HKUST-1 metal-organic framework nanoparticle/graphene oxide nanocomposite aerogels for CO2and CH4Adsorption and separation
Rosado, Albert (Institut de Ciència de Materials de Barcelona)
Borrás Caballero, Alejandro (Institut de Ciència de Materials de Barcelona)
Fraile, Julio (Institut de Ciència de Materials de Barcelona)
Navarro, Jorge A. R. (Universidad de Granada. Departamento de Química Inorgánica)
Suárez-García, Fabián (Consejo Superior de Investigaciones Científicas (Espanya). Instituto de Ciencia y Tecnología del Carbono)
Stylianou, Kyriakos C. (Oregon State University. Department of Chemistry)
Lopez-Periago, Ana M. (Institut de Ciència de Materials de Barcelona)
Giner Planas, José (Institut de Ciència de Materials de Barcelona)
Domingo, Concepción (Institut de Ciència de Materials de Barcelona)
Yazdi, Amirali (Institut de Ciència de Materials de Barcelona)

Data:	2021
Resum:	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.
Ajuts:	Agencia Estatal de Investigación PID2020-115631GB-I00 Ministerio de Ciencia e Innovación CEX2019-000917-S Agencia Estatal de Investigación PID2019-106832RB-I00 Agencia Estatal de Investigación RTI2018-100832-B-I00 Agencia Estatal de Investigación CTQ2017-83632 Agencia Estatal de Investigación CTQ2017-84692-R Agencia Estatal de Investigación CTQ2016-75150-R Ministerio de Economía y Competitividad SEV-2015-0496
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Llengua:	Anglès
Document:	Article ; recerca ; Versió acceptada per publicar
Matèria:	Supercritical CO2 ; Composite materials ; HKUST-1/GO ; Aerogels ; Gas adsorption ; Gas separation
Publicat a:	ACS applied nano materials, Vol. 4, issue 11 (November 2021) , p. 12712-12725, ISSN 2574-0970

DOI: 10.1021/acsanm.1c03301

Article 42 p, 1.7 MB

Material suplementari 13 p, 1.3 MB

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