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A gas phase analysis technique applied to in-situ studies of gas-solid interactions
KTH, Skolan för industriell teknik och management (ITM), Materialvetenskap.
KTH, Skolan för industriell teknik och management (ITM), Materialvetenskap.
2007 (Engelska)Ingår i: Journal of materials science. Materials in electronics, ISSN 0957-4522, E-ISSN 1573-482X, Vol. 47, nr 10, s. 3440-3453Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

An ultrahigh vacuum technique using mass spectrometry for in-situ investigations of gas-solid interactions is described in this paper. Examples of chemical reactions (oxidation, hydration) between solids and gas mixtures, dissociation of gases on solid surfaces, outgassing of solid materials and permeation of gases through membranes are discussed where the experimental arrangement is explained in detail. This Gas Phase Analysis (GPA) technique can be used at temperatures from room temperature to 1200 degrees C and at pressures up to 1 atm. Aspects related to sample preparation, isotopic gas mixture selection, data acquisition, calibration and interpretation of the experimental data are also addressed.

Ort, förlag, år, upplaga, sidor
2007. Vol. 47, nr 10, s. 3440-3453
Nyckelord [en]
temperature oxidation-kinetics, oxide-growth mechanisms, mass-spectrometry, scale adherence, metal-oxides, hydrogen, o-2, chromium, iron, dissociation
Nationell ämneskategori
Teknik och teknologier
Identifikatorer
URN: urn:nbn:se:kth:diva-6093DOI: 10.1007/s10853-006-1023-6ISI: 000246618700023Scopus ID: 2-s2.0-34249057540OAI: oai:DiVA.org:kth-6093DiVA, id: diva2:10704
Anmärkning
Conference: Workshop on Size-dependent Effects in Materials for Environmental Protection and Energy Application. Varna, BULGARIA. MAY 25-27, 2006 Tillgänglig från: 2006-09-08 Skapad: 2006-09-08 Senast uppdaterad: 2017-12-14Bibliografiskt granskad
Ingår i avhandling
1. Modified oxygen and hydrogen transport in Zr-based oxides
Öppna denna publikation i ny flik eller fönster >>Modified oxygen and hydrogen transport in Zr-based oxides
2006 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

Most metals and alloys in the presence of oxygen and moisture will instantaneously react and form a thin (2-5 nm) surface oxide layer. For further reaction to occur, oxygen ions and/or metal cations often diffuse through the already formed oxide layer. The corrosion resistance of a metal in aggressive environments at high temperatures depends on the properties of the surface oxide scale.

Zirconium-based alloys represent the main structural materials used in water-cooled nuclear reactors. For these materials, the formation of a thin, adherent oxide scale with long-term stability in high temperature water/steam under irradiation conditions, is crucial. In this thesis, the transport of oxygen and hydrogen through Zr-based oxide scales at relevant temperatures for the nuclear industry is investigated using isotopic gas mixtures and isotope-monitoring techniques such as Gas Phase Analysis and Secondary Ion Mass Spectrometry.

Porosity development in the oxide scales generates easy diffusion pathways for molecules across the oxide layer during oxidation. A considerable contribution of molecular oxygen to total oxygen transport in zirconia has been observed at temperatures up to 800°C. A novel method for evaluation of the gas diffusion, gas concentration and effective pore size of oxide scales is presented in this thesis. Effective pore sizes in the nanometer range were found for pretransition oxides on Zircaloy-2. A mechanism for densification of oxide scales by obtaining a better balance between inward oxygen and outward metal transport is suggested. Outward Zr transport can be influenced by the presence of hydrogen in the oxide and/or metal substrate. Inward oxygen transport can be promoted by oxygen dissociating elements such as Fe-containing second phase particles. The results suggest furthermore that a proper choice of the second-phase particles composition and size distribution can lead to the formation of dense oxides, which are characterized by low oxygen and hydrogen uptake rates during oxidation.

Hydrogen uptake in Zr-based materials during oxidation in high temperature water/steam can generate degradation due to the formation of brittle hydrides in the metal substrate. A promising method for the suppression of hydrogen uptake has been developed and is presented in this thesis.

Ort, förlag, år, upplaga, sidor
Stockholm: KTH, 2006. s. 48
Nyckelord
Zirconia, Zirconium, Zircaloy, hydrogen and oxygen diffusion, SPP, oxygen dissociating elements, oxidation, dissociation, hydration, CO adsorption, molecular transport, porosity.
Nationell ämneskategori
Materialteknik
Identifikatorer
urn:nbn:se:kth:diva-4095 (URN)91-7178-429-2 (ISBN)
Disputation
2006-09-22, F3, Lindstedtsvägen 26, Stockholm, 10:00
Opponent
Handledare
Anmärkning
QC 20100629Tillgänglig från: 2006-09-08 Skapad: 2006-09-08 Senast uppdaterad: 2011-10-05Bibliografiskt granskad

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Anghel, ClaraDong, Qian
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