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Materials at High Temperatures (2005), 22(3/4)

 

 

Phase identification of oxide scale on low carbon

steel

S. Birosca and R. L. Higginson

IPTME: Institute of Polymer Technology and Materials Engineering, Loughborough

University, Loughborough, Leicestershire LE11 3TU, UK

 

ABSTRACT

The classical model of iron oxide scale layers; wu¨stite, magnetite and hematite, is more complicated

in reality and its properties change with the factors that affect their development, such as time,

temperature, alloying elements in the steel and oxidation environment. An understanding of the oxide

scale formation and its properties can only be achieved by careful examination of the scale

microstructure. Throughout this study, electron back-scatter diffraction (EBSD) has proved to be a

powerful technique for verifying the individual phases in the oxide scale accurately. The results show

that EBSD can be used to give a complete characterisation of the oxide scale formed on low carbon

steel surface. Microstructural features such as grain size, shape and grain boundary characteristics

have been successfully determined and analysed.

 

Keywords: steel, oxidation, phase identification, electron back-scatter diffraction

 

 

 

 

In-situ scanning electron microscopy and electron

backscatter diffraction investigation on the

oxidation of pure iron

B. Poter, I. Parezanovic´ and M. Spiegel

Max-Planck-Institute for Iron Research Ltd., Dusseldorf, Germany

 

ABSTRACT

a-iron samples, with a 4 to 6 nm oxide layer on top of the surface due to preparation, were oxidised in

situ within a scanning electron microscopy equipped with electron back-scatter diffraction. At 773 and

973 K, two different growth mechanisms during the initial stage of iron oxide formation could be

observed, layer-by-layer growth at 773K and island growth at 973 K. The growth mechanism at

973K is correlated to the formation of a thin layer of Fe1_XO (wu¨stite) prior to Fe3O4 (magnetite)

crystallisation whereas at 773K only magnetite was found as newly grown oxide. Magnetite showed

a strong epitaxial relationship to a-iron with its {111} plane growing preferentially on the {110}

plane of iron.

 

Keywords: oxidation of pure iron, Fourier electron-electron back-scatter diffraction

 

 

 

 

Effect of water vapour on growth and adherence

of chromia scales formed on Cr in high and low

pO2-environments at 1000 and 1050_C

M. Michalik, M. Ha¨ nsel, J. Zurek, L. Singheiser and W.J. Quadakkers

Forschungszentrum Julich GmbH, IWV-2, PB 1913, 52425 Julich, Germany

 

ABSTRACT

The oxidation behaviour of pure Cr at 1000 and 1050_C was studied in Ar–O2 and Ar –H2–H2O

mixtures. It was found that in the low-pO2 gases the oxide scales exhibited higher growth rates than

in the high-pO2 gases. The scales formed in the low-pO2 gases showed substantially better adherence

during cooling, than scales formed in the high-pO2 gases. These differences in growth rate and

adherence can be correlated with differences in size and location of the in-scale voids formed during

the isothermal exposure. Exposures in Ar-O2-H2O mixtures revealed that the differences in scale

growth rates as well as in scale void formation and growth are not primarily related to differences in

the oxygen partial pressure of the atmosphere but to the presence of water vapour in the test gas. At

sufficiently high H2OyO2-ratios, water vapour promotes oxide formation at the scaleymetal interface

thereby suppressing excessive growth of existing voids, and also as a consequence improved scale

adherence. Whether the enhancement of inward scale growth is related to transport of H2O- or H2-

molecules or due to OH_ ions, cannot be derived with certainty from the present results.

 

Keywords: water vapour, growth and adherence of chromia scales, Cr, p(O2)-environments

 

 

 

 

Influence of the oxidation environment on scale

morphology and oxidation rate of Fe–22Cr

Anette N. Hansson and Marcel A.J. Somers

Department of Manufacturing Engineering and Management, Technical University of

Denmark, Kemitorvet b. 204, DK-2800 Kgs. Lyngby, Denmark

 

ABSTRACT

The oxidation behaviour of a commercial Fe –Cr alloy with 22 wt% Cr was investigated at 1173K in

Ar – 9 H2 with 1% H2O (pO2 ¼ 9:8610_19), in air with 1% H2O (pO2 ¼ 0:208), and in a

combination of the two atmospheres. The oxide morphology was investigated with X-ray diffraction

and scanning electron microscopy. The oxide layer consisted of MnCr2O4 on top of Cr2O3.

Small oxide whiskers were present at the surface after oxidation in Ar – 9 H2 with 1% H2O but not

after oxidation in air with 1% H2O. For samples initially oxidised in air with 1% H2O, the

oxideyalloy interface was wrinkled and covered with a SiO2 layer. SiO2 particles had developed at

a rather flat oxideyalloy interface for samples initially oxidised in Ar – 9% H2 with 1% H2O. The

results obtained can be explained assuming that oxide growth occurs by cation diffusion only in Ar – 9

H2 with 1% H2O, whereas both cation and anion diffusion contribute to the growth in airyH2O.

 

Keywords: oxidation environment, scale morphology, oxidation rate, Fe– 22Cr

 

 

 

 

Microstructural investigation of the effect of water

vapour on the oxidation of alloy 353 MA in oxygen

at 700 and 900_C

T. Jonssona, S. Canovica, F. Liua, H. Astemanb, J.-E. Svenssonb, L.-G. Johanssonb and M. Halvarssona

aDepartment of Applied Physics, Chalmers University of Technology, SE-412 96 Go¨ teborg, Sweden

bDepartment of Environmental Inorganic Chemistry, Chalmers University of Technology, SE-412 96 Go¨ teborg, Sweden

 

ABSTRACT

The objective of this work was to study the impact of water vapour on the corrosion behaviour of the

austenitic stainless steel 353MA at 700 and 900_C through a detailed microstructural characterisation

of the oxide scales formed, after 168 hours, in O2 and O2 with 40% H2O. The oxidized samples were

investigated by scanning electron microscope/energy dispersive X-ray, focused ion beam and

transmission electron microscope/energy dispersive X-ray. At 700_C 353MA forms a Cr-rich

protective (Fe,Cr)2O3 oxide scale, with some silica at the oxideymetal interface. Breakaway oxidation

occurs in H2OyO2 mixtures because the oxide scale is depleted in Cr due to the formation of

CrO2(OH)2(g). However, the microstructural investigation indicated that a healing Cr-rich oxide layer

formed beneath the Fe-rich oxide after some time. This could be a result of the high CryFe ratio of

353MA. The behaviour at 900_C was different. In spite of the loss of Cr from the oxide scale,

breakaway oxidation did not occur, i.e. the oxide scale remained protective. The microstructural

investigation showed a thick, almost continuous silica layer at the oxideymetal interface, which may

act as a diffusion barrier at the higher temperature.

 

Keywords: 353MA, high temperature oxidation, water vapour effect, silica, microstructure, scanning electron

microscope, focused ion beam, transmission electron microscope, energy dispersive X-ray

 

 

 

 

Oxidation of potential SOFC interconnect

materials, Crofer 22 APU and Avesta 353 MA, in

dry and humid air studied in situ by X-ray diffraction

Maria Jose Garcia-Vargasa, Laurent Lelaita, Vladislav Kolarikb, Harald Fietzekb and Maria del Mar Juez-Lorenzob

aEdFyEIfER (European Institute For Energy Research), Karlsruhe, Germany

bFraunhofer-Institut fu¨ r Chemische Technologie (ICT), Pfinztal, Germany

 

ABSTRACT

Several stainless steels have been developed for the use as interconnect materials in solid oxide fuel

cells in order to reduce costs, while maintaining the required performance. The materials however, are

subjected to humid air, at high temperatures up to 800_C leading to enhanced oxidation. High

temperature X-ray diffraction, combined with field emission – scanning electron microscopy, has been

applied to study in situ the influence of water vapour on the chromia scale formation on the ferritic

Crofer 22 APU and the austenitic Avesta 353 MA alloys in comparison to their dry air oxidation

behaviour. Both materials form at 800_C, during the first 100 h exposure, Cr2O3 and MnCr2O4, the

latter mostly in the surface region of the oxide scale. Additionally, Crofer 22 APU forms internal

Al2O3 precipitates, while on Avesta 353 MA a SiO2 layer is found beneath the outer oxide scale.

High temperature XRD indicates stress formation and relaxation in the Cr2O3 scale formed in humid

air, especially for Crofer 22 APU.

 

Keywords: SOFC interconnect, oxidation in dry and humid air, in situ X-ray diffraction

 

 

 

 

Effect of component thickness on lifetime and

oxidation rate of chromia forming ferritic steels in

low and high pO2 environments

P. Huczkowski, S. Ertl, J. Piron-Abellan, N. Christiansena, T.Ho¨ flerb, V. Shemet, L. Singheiser and W.J. Quadakkers

Forschungszentrum Ju¨ lich, Institute for Materials and Processes in Energy Systems, D-52425 Ju¨ lich, Germany

aHaldor Topsøe AyS, Lyngby, Denmark, and bBMW, Munich, Germany

 

ABSTRACT

Long term oxidation tests were carried out with a high-Cr ferritic steel at 800_C and 900_C in

simulated cathode and anode gas of a solid oxide fuel cell (air and an AryH2yH2O mixture

respectively). It was found that with decreasing sample thickness the life time of the steel decreases

due to breakaway phenomena. This effect is caused by faster exhaustion of the chromium reservoir

from the bulk alloy in the case of thinner components. During air exposure the oxidation rates

increase with decreasing specimen thickness and this has to be taken into account in the calculation of

the Cr-reservoir exhaustion. This thickness dependence is not found during the exposures in simulated

anode gas. Hence, especially for thin walled components, the oxidation rates in anode gas are

substantially smaller and thus the life times are longer than during air exposure. The differences in

oxidation behaviour in the two environments are discussed on the basis of scale formation

mechanisms involving microcrack formation in the surface oxide scale and depletion of major and

minor alloying additions in the bulk alloy.

 

Keywords: high temperature oxidation, ferritic steels, chromia scales, breakaway oxidation

 

 

 

 

Long term steam oxidation of TP 347H FG in

power plants

A.N. Hanssona, L. Korcakovab, J. Halda and M. Montgomerya

aDepartment of Manufacturing Engineering and Management, Technical University of Denmark, Kemitorvet b. 204, DK-2800 Kgs. Lyngby, Denmark

bMaterials Research Department, Risø National Laboratory, Frederiksborgvej 399, PO Box 49, DK-4000 Roskilde, Denmark

 

ABSTRACT

The long term oxidation behaviour of TP 347H FG at ultra supercritical steam conditions was

assessed by exposing the steel in test superheater loops in a Danish coal-fired power plant. The

steamside oxide layer was investigated with scanning electron microscopy and energy dispersive Xray

diffraction in order to reveal the effect of oxidation time and temperature on the microstructure.

A double layered oxide formed during steam oxidation. The morphology of the inner Crcontaining

layer was influenced by the oxidation temperature. At temperatures below 585_C, it

consisted of regions of Fe –Ni – Cr spinel surrounded by Fe –Cr oxide. At higher temperatures almost

the entire inner oxide layer was composed of Fe –Cr oxide. Possible mechanisms for the oxide growth

are discussed and it is suggested that faster Cr transport within the alloy at higher temperatures

explains the change in morphology.

The thickness of the inner oxide layer appeared to be independent of oxidation time and

temperature for exposes less than 30 000 h; however, after 57 554 h, the thickness had increased

significantly at the lowest temperatures.

 

Keywords: long term steam oxidation, TP 347H FG, power plants

 

 

 

 

Role of nickel in the oxidation of Fe–Cr–Ni alloys

in air –water vapour atmospheres

R.F.A. Pettersson, J. Enecker and L. Liu

Corrosion and Metals Research Institute, Drottning Kristinas va¨g 48, 114 28 Stockholm, Sweden

 

ABSTRACT

A series of experimental austenitic alloys has been produced in which the nickel content ranges from

14 to 43%, with constant levels of 20%Cr, 1%Mn and 0.5%Si. A combination of isothermal,

discontinuous and cyclic oxidation testing has been used to elucidate the performance in dry air and

in air with 10%, 45% or 62% water vapour at 700_C and 1000_C. Evaluation was by means of

thermogravimetry, surface analysis with glow discharge optical emission spectroscopy and scanning

electron microscopy.

Nickel is shown to have several roles: it accelerates the kinetics of chromia formation yet

suppresses chromia spallation at 700_C. At 1000_C, it strongly decreases the breakaway oxidation and

spalling associated with iron oxide formation. This effect is particularly marked in environments

containing water vapour, where the material loss may be decreased 10-fold by an increase in the

nickel content. Results correlate to thermodynamic and kinetic data which show nickel to increase the

chromium activity and diffusivity in the alloy.

 

Keywords: nickel, Fe– Cr–Ni alloys, air – water vapour atmospheres

 

 

 

 

High temperature oxidation behavior of a

Mo– 3Si –1B(wt%) alloy

D.A. Helmick, G.H. Meier and F.S. Pettit

Department of Materials Science and Engineering, University of Pittsburgh, Pittsburgh, PA 15261, USA

 

ABSTRACT

Molybdenum base alloys with the addition of small amounts of silicon (2 – 4.5 wt.%) and boron

(~1 wt.%) can form a passivating layer protecting the alloy from further rapid oxidation. When such

molybdenum base alloys are exposed to oxidizing environments at high temperatures, a borosilicate

glass layer can form that will reduce the transport of oxygen to the alloy to limit further oxidation.

Oxidation is then controlled by diffusion through the borosilicate glass layer. The focus of this

research was to study the mechanisms and kinetics of high temperature oxidation of a Mo–Si –B

alloy. The base alloy has a composition of Mo – 3Si – 1B (wt.%) and was studied in a variety of gas

environments over a range of temperatures in order to elucidate the critical factors that allow it to

develop a protective borosilicate glass layer. The borosilicate glass layer is protective when no

continuous channels exist in the layer extending from the gas interface to the alloy interface. The

borosilicate layer is believed to contain channels in the early stages of development and the

elimination of the channels is obtained by appropriate control of the temperature and gas flow

conditions whereby MoO3 is removed via vaporization while the borosilicate viscosity is not

increased due to loss of B2O3. Once the borosilicate layer is continuous and free of channels,

subsequent oxidation occurs by inward diffusion of oxygen and the outward diffusion of molybdenum

through this layer with vaporization of MoO3 occurring at the gasyborosilicate layer interface, and

MoO2 and additional borosilicate forming at the alloyyMoO2 interface.

 

Keywords: high temperature oxidation behavior, Mo – 3Si – 1B(wt.%) alloy

 

 

 

 

The halogen effect for improving the oxidation

resistance of TiAl-alloys

A. Donchev, H.-E. Zschau and M. Schu¨ tze

DECHEMA e.V Karl-Winnacker-Institut, Theodor-Heuss-Allee 25, D-60486 FrankfurtyMain, Germany

 

ABSTRACT

Alloys based on TiAl intermetallics are potential candidates for high temperature applications in e.g.

aero engines or automotive engines because of their low specific weight and good high temperature

strength. To improve their oxidation resistance at temperatures up to 1000_C the halogen effect offers

an innovative and cost-effective way. The addition of small amounts of halogens into the surface

leads to the preferential formation of gaseous aluminium halides which are oxidised to aluminium

oxide during their outward migration forming a dense, protective and slowly growing alumina scale

on the surface. In this paper two methods were used to apply halogens to the surface, ion implantation

(F and Cl) and a liquid phase process (F). Ion beam analysis with detection limits in the ppm-range

was applied to quantify the needed amount of halogens to achieve the halogen effect. Thermocyclic

oxidation experiments at 900_C were performed in laboratory air and wet air. Depth concentration

profiles of fluorine were measured by PIGE within the first 1.4 mm without destruction of the sample

before and after oxidation. Furthermore, the loss of fluorine during heating up and oxidation was

measured characterising the stability of the effect. Simultaneous RBS-measurements of the O-, Aland

Ti-depth profiles prove the formation and growth of an almost pure alumina scale. Correlation

with the fluorine profiles validates the proposed model for the halogen effect. Furthermore,

metallographic methods, REM, EPMA, AES and the proton micro beam (PIXE) were applied to

study cross-sections. A virtually pure alumina scale was found after F-treatment and oxidation up to

1500 hours at 900 – 1000_C in air. The fluorine depth profiles after ion implantation and liquid phase

treatment, respectively, show similar levels for both methods before and after oxidation. The

development of the fluorine interfacial concentration underneath the oxide scale as a function of

oxidation time and temperature was recorded. The results are discussed in the light of the existing

model considerations on the halogen effect and with regards to differences in the behaviour between

F- and Cl-doping.

 

Keywords: halogen effect, oxidation resistance, TiAl-alloys

 

 

 

 

Photoelectrochemical and Raman imaging studies

of chemical and mechanical properties of thermally

grown titanium oxide scales

Y. Woutersa, A. Galeriea, P. Bouvierb, M. Mermouxb and J.-P. Petitb

aLaboratoire de Thermodynamique et de Physicochimie Me´ tallurgiques, UMR CNRSyINPGyUJF 5614

bLaboratoire d’Electrochimie et de Physicochimie des Mate´ riaux et des Interfaces, UMR CNRSyINPGyUJF 5631

Institut National Polytechnique de Grenoble – Ecole Nationale Superieure d’Electrochimie et d’Electrome´ tallurgie de Grenoble,

BP 75 Domaine Universitaire, F – 38402 Saint-Martin-d’He` res Cedex France

 

ABSTRACT

The present work focuses on thin TiO2 scales (up to 3 mm). The use of both micro-photoelectrochemistry

(MPEC) and Raman imaging aims to get chemical and mechanical information at a

micron scale. In particular, the MPEC technique allows images of the history of strain and adhesion

levels of the oxideymetal interface to be realised. A set of photocurrent images recorded at different

applied potentials allows different images to be constructed, Structural Quality Image (SQI) and

Interface Cohesion Image (ICI). In addition, Raman spectroscopy images the chemical nature of the

scale, topography of the surface and local stress level in the scale. Combining both techniques is a

powerful tool in elucidating the mechanisms of thermal oxidation.

 

Keywords: thermal oxidation, titanium, MicroPhotoElectroChemistry (MPEC), Raman spectroscopy

 

 

 

 

Effects of Pt on the short-term oxidation behavior

of g-Niþ+g-Ni3Al alloys

Shigenari Hayashia and Brian Gleesonb

aDivision of Materials Science and Engineering, Hokkaido University, N13, W8, Kitaku, Sapporo, 060-8628, Japan