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New Methods for the Determination of Sorption Capacities and Sorption-Related Properties of Intact Rock
KTH, Skolan för kemivetenskap (CHE), Kemiteknik, Kemisk apparatteknik. (Kemisk apparatteknik)
2009 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Ort, förlag, år, upplaga, sidor
Stockholm: KTH , 2009. , s. viii, 77
Serie
Trita-CHE-Report, ISSN 1654-1081 ; 2009:19
Nationell ämneskategori
Kemiteknik
Identifikatorer
URN: urn:nbn:se:kth:diva-10636ISBN: 978-91-7415-332-3 (tryckt)OAI: oai:DiVA.org:kth-10636DiVA, id: diva2:222404
Disputation
2009-06-12, K1, KTH, Teknikringen, Stockholm, 10:00 (Engelska)
Opponent
Handledare
Anmärkning
QC 20100622Tillgänglig från: 2009-06-08 Skapad: 2009-06-08 Senast uppdaterad: 2011-10-10Bibliografiskt granskad
Delarbeten
1. Determination of sorption properties of intact rock samples: New methods based on electromigration
Öppna denna publikation i ny flik eller fönster >>Determination of sorption properties of intact rock samples: New methods based on electromigration
2009 (Engelska)Ingår i: Journal of Contaminant Hydrology, ISSN 0169-7722, E-ISSN 1873-6009, Vol. 103, nr 3-4, s. 71-81Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Two new methods for determining sorption coefficients in large rock samples have been developed. The methods use electromigration as a means to speed up the transport process, allowing for fast equilibration between rock sample and tracer solution. An electrical potential gradient acts as a driving force for transport in addition to the concentration gradient and forces the cations through the rock sample towards the cathode. The electrical potential gradient induces both electromigration and electroosmotic flow with a resulting solute transport that is large compared to diffusive fluxes. In one of the methods, the solute is driven through the sample and collected at the cutlet side. In the other, simpler method, the rock sample is equilibrated by circulating the solute through the sample. The equilibration of rock samples, up to 5 cm in length, with an aqueous solution has been accomplished within days to months. Experiments using cesium as a sorbing tracer yield results consistent with considerably more time demanding in-diffusion experiments. These methods give lower distribution coefficients than those obtained using traditional batch experiments with crushed rock. (C) 2008 Elsevier B.V. All rights reserved.

Nyckelord
K-d, Ion exchange, Retardation, Sorption, Electromigration, Cesium, Granite, Intact rock, MIGRATION BEHAVIOR, UNIFIED MODEL, POROUS-MEDIA, BOOM-CLAY, CONDUCTIVITY, DIFFUSIVITY, STRONTIUM, MEMBRANE, MINERALS
Nationell ämneskategori
Kemiteknik
Identifikatorer
urn:nbn:se:kth:diva-13628 (URN)10.1016/j.jconhyd.2008.09.006 (DOI)000263009100001 ()2-s2.0-58149165041 (Scopus ID)
Anmärkning
QC 20100622Tillgänglig från: 2010-06-22 Skapad: 2010-06-22 Senast uppdaterad: 2017-12-12Bibliografiskt granskad
2. Specific surface area determinations on intact drillcores and evaluation of extrapolation methods for rock matrix surfaces
Öppna denna publikation i ny flik eller fönster >>Specific surface area determinations on intact drillcores and evaluation of extrapolation methods for rock matrix surfaces
2009 (Engelska)Ingår i: Journal of Contaminant Hydrology, ISSN 0169-7722, E-ISSN 1873-6009, Vol. 110, nr 1-2, s. 1-8Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Permanent storage of spent nuclear fuel in crystalline bedrock is investigated in several countries. For this storage scenario, the host rock is the third and final barrier for radionuclide migration. Sorption reactions in the crystalline rock matrix have strong retardative effects on the transport of radionuclides. To assess the barrier properties of the host rock it is important to have sorption data representative of the undisturbed host rock conditions. Sorption data is in the majority of reported cases determined using crushed rock. Crushing has been shown to increase a rock samples sorption capacity by creating additional surfaces. There are several problems with such an extrapolation. In studies where this problem is addressed, simple models relating the specific surface area to the particle size are used to extrapolate experimental data to a value representative of the host rock conditions. In this article, we report and compare surface area data of five size fractions of crushed granite and of 100 mm long drillcores as determined by the Brunauer Emmet Teller (BET)-method using N-2-gas. Special sample holders that could hold large specimen were developed for the BET measurements. Surface area data on rock samples as large as the drillcore has not previously been published. An analysis of this data show that the extrapolated value for intact rock obtained from measurements on crushed material was larger than the determined specific surface area of the drillcores, in some cases with more than 1000%. Our results show that the use of data from crushed material and current models to extrapolate specific surface areas for host rock conditions can lead to over estimation interpretations of sorption ability. The shortcomings of the extrapolation model are discussed and possible explanations for the deviation from experimental data are proposed.

Nyckelord
BET, Specific surface area, Crystalline rock, Disturbed zone, Rock matrix, MINERALS, SORPTION, SAMPLES, DIFFUSIVITY, STRONTIUM, POROSITY, GRANITE, CESIUM, ZONE
Nationell ämneskategori
Kemiteknik
Identifikatorer
urn:nbn:se:kth:diva-13629 (URN)10.1016/j.jconhyd.2009.05.003 (DOI)000271836600001 ()2-s2.0-71749092641 (Scopus ID)
Anmärkning
QC 20100622Tillgänglig från: 2010-06-22 Skapad: 2010-06-22 Senast uppdaterad: 2017-12-12Bibliografiskt granskad
3. Rapid surface area determination of crystalline rock using impedance spectroscopy
Öppna denna publikation i ny flik eller fönster >>Rapid surface area determination of crystalline rock using impedance spectroscopy
(Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
Nyckelord
Impedance spectroscopy, complex conductivity, specific surface area, rock matrix
Nationell ämneskategori
Kemiteknik
Identifikatorer
urn:nbn:se:kth:diva-13630 (URN)
Anmärkning
QC 20100622. Submitted to Journal of Geophysical Research - Solid EarthTillgänglig från: 2010-06-22 Skapad: 2010-06-22 Senast uppdaterad: 2011-10-10Bibliografiskt granskad
4. Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
Öppna denna publikation i ny flik eller fönster >>Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
2008 (Engelska)Ingår i: Radiochimica Acta, ISSN 0033-8230, E-ISSN 2193-3405, Vol. 96, nr 9-11, s. 673-677Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

In general sorption coefficients, K-d cat ion exchange capacity, CEC, and BET surface areas are measured on crushed rock samples because it is very time consuming to measure K-d and CEC on larger rock pieces as it takes a long time for the sorbing species to penetrate into and equilibrate a large sample. Also conventional sample holders for BET measurements are too small to hold a large sample. We have manufactured large sample holders for BET measurements and modified the equipment so that it is possible to measure BET surface areas on samples with 50 mm diameter and LIP to 100 mm length. Results are presented for intact pieces and compared to results on crushed material from the same drillcore. For K-d and CEC measurements we have developed a technique and equipment by which ions can be made to rapidly intrude into and equilibrate the internal surfaces of the same size samples as mentioned above. The method is based on electro-migration where the sample is placed between two vessels one with an anode and other with a cathode. The electric potential gradient drives the ions into and through the sample very much faster than molecular diffusion does. With Cs as the sorbing ion a few weeks were sufficient to equilibrate the 50 mm long sample. In previous diffusion experiments it took more than a year to equilibrate a 15 mm thick sample. A special mixing technique eliminates the development of low and high PH in the electrode compartments. K-d results from measurements on an intact drillcore are presented and comparison is made with results obtained on crushed material from the same bore core. The results from the sorption experiments are compared with the results from the BET surface area determinations in an attempt to evaluate the use of the BET surface area as a proxy for sorption behaviour.

Nyckelord
Sorption, Electromigration, Crystalline rock, Granite, BET-surface area, Specific surface area, ROCK
Identifikatorer
urn:nbn:se:kth:diva-13631 (URN)10.1524/ract.2008.1552 (DOI)000261096500023 ()2-s2.0-56649094297 (Scopus ID)
Anmärkning
QC 20100622Tillgänglig från: 2010-06-22 Skapad: 2010-06-22 Senast uppdaterad: 2017-12-12Bibliografiskt granskad

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