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The Porous Network and its Interface inside Geopolymers as a Function of Alkali Cation and Aging

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dc.title The Porous Network and its Interface inside Geopolymers as a Function of Alkali Cation and Aging en
dc.contributor.author Melar, Jaroslav
dc.contributor.author Renaudin, Guillaume
dc.contributor.author Leroux, Fabrice
dc.contributor.author Hardy-Dessources, Adeline
dc.contributor.author Nedelec, Jean Marie
dc.contributor.author Taviot-Guého, Christine
dc.contributor.author Petit, Elodie
dc.contributor.author Steins, Prune
dc.contributor.author Poulesquen, Arnaud
dc.contributor.author Frizon, Fabien
dc.relation.ispartof Journal of Physical Chemistry C
dc.identifier.issn 1932-7447 Scopus Sources, Sherpa/RoMEO, JCR
dc.date.issued 2015
utb.relation.volume 119
utb.relation.issue 31
dc.citation.spage 17619
dc.citation.epage 17632
dc.type article
dc.language.iso en
dc.publisher American Chemical Society
dc.identifier.doi 10.1021/acs.jpcc.5b02340
dc.relation.uri http://pubs.acs.org/doi/full/10.1021/acs.jpcc.5b02340
dc.description.abstract A combination of original, powerful characterization techniques was used to make a thorough description of solid geopolymers and of the associated effect of varying the alkali cation source - NaOH, KOH, or CsOH - and aging for up to several years. More specifically, the local and pore structures were progressively determined from atomic local scale up to several nanometers by pair distribution function analysis (PDF), small-angle X-ray scattering (SAXS), and longer correlation concerning the pore network, and possible diffusion and accumulation phenomena were unraveled by thermoporosimetry and electrochemical impedance spectroscopy (EIS), respectively. These complementary observations resulted in a picture of an interface between the mineral and the porous network that was correlated to the solvated alkali cation present in the porous solution. After a short time of a few months, the Na-based geopolymer was found to exhibit a smooth interface built up from small "elementary"particles. This contrasted with the K- and Cs-based geopolymers, which presented developed interfaces arising from hierarchically organized smooth particles forming aggregates of fractal outer surface. This striking difference unraveled by SAXS and EIS is ascribed for the Na geopolymer to the contact of the solvated Na(H<inf>2</inf>O)<inf>x</inf>+ cations with the amorphous mineral surface. The K(H<inf>2</inf>O)<inf>x</inf>+ and Cs(H<inf>2</inf>O)<inf>x</inf>+ solvated cations were an integral part of the porous solution, without direct contact with the mineral surface, thus leading to apparently rough interfaces. Dewatering occurred with time, mostly impacting the Na series. Overall, we obtained a detailed picture of the geopolymer series and their changes in time. The environment generated around the kosmotropic (order-making) Na+ alkali cation was more prone to change upon aging toward a non-Debye type relaxation than the initially developed interface supplied by the chaotropic Cs+ alkali cation, which was found to be relatively stable after 5 years. © 2015 American Chemical Society. en
utb.faculty Faculty of Technology
dc.identifier.uri http://hdl.handle.net/10563/1005287
utb.identifier.obdid 43873431
utb.identifier.scopus 2-s2.0-84938704067
utb.identifier.wok 000359332200014
utb.source j-wok
dc.date.accessioned 2015-09-09T15:16:26Z
dc.date.available 2015-09-09T15:16:26Z
dc.description.sponsorship ENSCCF (Ecole Nationale Superieure de Chimie de Clermont-Ferrand)
utb.contributor.internalauthor Melar, Jaroslav
utb.fulltext.affiliation Jaroslav Melar †,∥, Guillaume Renaudin *†,§, Fabrice Leroux ‡,§, Adeline Hardy-Dessources ‡,§, Jean-Marie Nedelec †,§, Christine Taviot-Gueho ‡,§, Elodie Petit ‡,§, Prune Steins ⊥, Arnaud Poulesquen ⊥, Fabien Frizon ⊥ † Université Clermont Auvergne, ENSCCF, Institut de Chimie de Clermont-Ferrand, BP 10448, 63000 Clermont-Ferrand, France ‡ Université Clermont Auvergne, Université Blaise Pascal, Institut de Chimie de Clermont-Ferrand, BP 10448, 63000 Clermont-Ferrand, France § CNRS, UMR 6296, 63177 Aubiere, France ∥ Department of Environment Protection Engineering, Tomas Bata University in Zlin, Faculty of Technology, 76272 Zlin, Czech Republic ⊥CEA, DEN, DTCD/SPDE/LCFI-Marcoule, 30207 Bagnols-sur-Ceze, France
utb.fulltext.dates Received: March 10, 2015 Revised: July 9, 2015 Published: July 9, 2015
utb.fulltext.faculty Faculty of Technology
utb.fulltext.ou Department of Environmental Protection Engineering
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