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Selective sulfur dioxide adsorption on crystal defect sites on an isoreticular metal organic framework series

[PDF] RodriguezAlbelo_DioxideAdsorption.pdf (1.989Mb)
Identificadores
URI: http://hdl.handle.net/10481/45375
DOI: 10.1038/ncomms14457
ISSN: 2041-1723
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Autor
Rodríguez-Albelo, L. Marleny; López-Maya, Elena; Harnad, Said; Ruiz-Salvador, A. Rabdel; Calero, Sofia; Rodríguez Navarro, Jorge Andrés
Editorial
Nature Publishing Group
Materia
Sulphur dioxide
 
Adsorption
 
Surface chemistry
 
Crystal
 
Isoreticular metal-organic
 
Properties
 
Fecha
2017
Referencia bibliográfica
Rodríguez-Albelo, L.M. ; et al. Selective sulfur dioxide adsorption on crystal defect sites on an isoreticular metal organic framework series. Nature Communications, 8: 14457 (2017). [http://hdl.handle.net/10481/45375]
Patrocinador
We thank generous funding from the European Research Council through an ERC Starting Grant (ERC2011-StG-279520-RASPA), the Spanish Ministry of Economy (CTQ2013-48396-P, CTQ2014-53486-R, CTQ2015-70135-REDT) and FEDER and Marie Curie IIF-625939 (LMRA) funding from European Union and Andalucía Region (FQM-1851).
Resumen
The widespread emissions of toxic gases from fossil fuel combustion represent major welfare risks. Here we report the improvement of the selective sulfur dioxide capture from flue gas emissions of isoreticular nickel pyrazolate metal organic frameworks through the sequential introduction of missing-linker defects and extra-framework barium cations. The results and feasibility of the defect pore engineering carried out are quantified through a combination of dynamic adsorption experiments, X-ray diffraction, electron microscopy and density functional theory calculations. The increased sulfur dioxide adsorption capacities and energies as well as the sulfur dioxide/carbon dioxide partition coefficients values of defective materials compared to original non-defective ones are related to the missing linkers enhanced pore accessibility and to the specificity of sulfur dioxide interactions with crystal defect sites. The selective sulfur dioxide adsorption on defects indicates the potential of fine-tuning the functional properties of metal organic frameworks through the deliberate creation of defects.
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