Papers by Author: Toshio Narita

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Authors: Toshio Narita, Takeshi Izumi, Takumi Nishimoto, Yoshimitsu Shibata, Kemas Zaini Thosin, Shigenari Hayashi
Abstract: To suppress interdiffusion between the coating and alloy substrate in addition to ensuring slow oxide growth at very high temperatures advanced coatings were developed, and they were classified into four groups, (1) the diffusion barrier coating with a duplex layer structure, an inner σ−(Re-Cr-Ni) phase as a diffusion barrier and outer Ni aluminides as an aluminum reservoir formed on a Ni based superalloy, Hastelloy X, and Nb-based alloy. (2) the up-hill diffusion coating with a duplex layer structure, an inner TiAl2 + L12 and an outer β-NiAl formed on TiAl intermetallic and Ti-based heat resistant alloys by the Ni-plating followed by high Al-activity pack cementation. (3) the chemical barrier coating with a duplex layer structure, an inner* γ + β + Laves three phases mixture as a chemical diffusion barrier and an outer Al-rich γ-TiAl as an Al reservoir formed by the two step Cr / Al pack process. (4) the self-formed coating with the duplex structure, an inner α-Cr layer as a diffusion barrier and an outer β-NiAl as an Al-reservoir on Ni-(2050)at% Cr alloy changed from the δ-Ni2Al3 coating during oxidation at high temperature. The oxidation properties of the coated alloys were investigated at temperatures between 1173 and 1573K in air for up to 1,000 hrs (10,000 hrs for the up-hill diffusion coating). In the diffusion barrier coating the Re-Cr-Ni alloy layer was stable, existing between the Ni-based superalloy (or Hastelloy X) and Ni aluminides containing 1250at%Al when oxidized at 1423K for up to 1800ks. It was found that the Re-Cr-Ni alloy layer acts as a diffusion barrier for both the inward diffusion of Al and outward diffusion of alloying elements in the alloy substrate. In the chemical barrier coating both the TiAl2 outermost and Al-rich γ-TiAl outer layers maintained high Al contents, forming a protective Al2O3 scale, and it seems that the inner, γ, β, Laves three phase mixture layer suppresses mutual diffusion between the alloy substrate and the outer/outermost layers.
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Authors: Toshio Narita
Abstract: The concept of the diffusion barrier coating system (DBC system) is summarized and the latest results are presented. The DBC system is comprised of alloy substrate/diffusion barrier/Al-reservoir/an external scale. Diffusion flux (JAl) of Al through the barrier layer will be given approximately by JAl = DAl x SAl x (d CAl/d x), where DAl and SAl are the diffusion coefficient and solubility limit of Al in the barrier layer, respectively as well as d CAl / d x is driving force given by the concentration difference across the barrier (d CAl) divided by the thickness of the barrier layer (d x). A slow diffusion flux can be obtained by using low values of DAl, SAl, or (d CAl /d x). Accordingly, a selection of a barrier layer with lower DAl and SAl is essential. A low driving force is also an important factor, and can be achieved by using lower CAl with a constant barrier layer thickness dx. At higher temperatures, however, the barrier layer can react with the alloy substrate and Al-reservoir layer, resulting in gradual degradation of the barrier layer. This means that the thickness dx of the barrier layer tends to decrease and may finally disappear. With decreasing thickness of the diffusion barrier layer, the driving force (dCAl/dx) will increase, and the effectiveness of the barrier layer will be eliminated. Therefore, it is essential to maintain a constant thickness of the barrier layer for long exposure time. Several types of the DBC system are proposed, a single barrier layer and triple-layers with g + g’ and g’ inserted among these barrier layers.
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Authors: Shigenari Hayashi, Mikihiro Sakata, Shigeharu Ukai, Toshio Narita
Abstract: High temperature oxidation / creep deformation behavior of a diffusion barrier coated Hastelloy-X alloy, with large grain size ~500μm, was investigated at 970°C in air with external tensile stress of 22.5, 27.5, 32, and 40MPa. The diffusion barrier coating formed on Hastelloy-X consisted of a duplex structure with an inner diffusion barrier layer of Re-Cr-Ni alloy, and an outer oxidation resistant layer of β-NiAl. Un coated bare Hastelloy-X alloy with same grain size was also examined under the same conditions for comparison. The composition of the as-coated diffusion barrier coating was (15~21)Ni, (33~37)Cr, (30~33)Re, (11~15)Mo, and (9~14)Fe. This composition corresponds to σ-phase in the Ni-Cr-Re ternary system, which is known as a topologically close packed, TCP phase. The composition of this diffusion barrier layer did not change during the experiment. The oxide scales formed after creep testing on the coated and un-coated alloy surfaces were needle-like θ-Al2O3, and Cr2O3 with small amount of FeCr2O4, respectively. Grain boundary oxidation was also found in the subsurface region of the un-coated alloy. The Al2O3 scale exhibited severe spallation, and many cracks were formed perpendicular to the stress direction. However, no spallation or cracks were observed in the Cr2O3. The creep rupture times for the diffusion barrier coated alloy were about 1.5 times longer than those for bare alloy at all creep stress conditions. The fracture surface after rupture indicates that fracture occurred along alloy grain boundaries in both the coated and un-coated alloy substrate. Many cavities and cracks were observed within the diffusion barrier coated alloy substrate. These cavities and cracks tended to propagate from the substrate toward the diffusion barrier layer, and then stopped at the Re-Cr-Ni / β-NiAl interface. Cracks formed in the un-coated alloy initiated at the tip of grain boundary oxides, and propagated into alloy substrate. However no major cavities were observed inside the alloy substrate. The stress index, n, for both specimens was about 6, and this indicates that the deformation mechanism of both samples was dislocation creep. These results suggest that the Re-Cr-Ni diffusion barrier layer acts as a barrier against the movement of dislocations at the interface with the alloy surface.
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Authors: S. Eni, Y. Wang, N. Hashimoto, Somei Ohnuki, Toshio Narita
Abstract: Cross-sectional structures of a Re-based diffusion barrier coating on Nb as ultra high temperature material were investigated in order to verify the crystalline structure and composition of the coated layer. Three types coating specimens were prepared by electroplating Re from an aqueous solution on an Nb substrate, followed by Cr-pack cementation in vacuum. The coating process produced three distinct layers; an outer Cr(Re) layer, an intermediate Re-Cr-Nb layer, and an inner Nb(Re) layer. A crystal structure of Cr(Re) and Nb(Re) layers possess similar single crystal bcc structure. The Re-Cr-Nb layer expected to act as a diffusion barrier between the substrate and the outer reservoir layer was comprised of cubic c phase and hexagonal Laves C14 phase. Moreover, several crystal defects such as dislocations and stacking faults as well as voids and cracks are observed in the coating specimen.
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Authors: Kosuke Saito, Shigenari Hayashi, Toshio Narita, Isao Iwanaga, Ryohei Tanaka
Abstract: A coating with a duplex layer structure, outer β-NiAl and inner σ-Re-Cr-Ni layers, was formed on the third generation Nb-5Mo-15W-16Si- 5Hf-5C alloy by using successively Re-pack cementation, electroplating of Re-Ni film, and Cr/Al pack cementation. The duplex layer coating changed during high temperature oxidation to form a coating with a four layer structure: an outermost Ni2Al3, an outer Ni, an inner σ-Re-Cr-Ni, and an innermost χ-Re-Nb. The Re-pack cementation was carried in an alumina crucible where the specimen was buried in Re metal powder, in vacuum at 1573K to form a Re film, and then a Re-Ni film was electroplated onto the Re-pack treated alloy. The coated alloy formed a protective α-Al2O3 scale when oxidized at 1573K in air for 14.4ks. It was concluded that the σ-Re-Cr-Ni phase can act as a diffusion-barrier against both inward Al diffusion and outward diffusion of alloying elements from the alloy substrate to the β-NiAl.
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Authors: Shigenari Hayashi, Toshio Narita, Brian Gleeson
Abstract: The early-stage oxidation behavior of γ '-Ni3Al-based alloys of composition (in at.%) Ni-22Al and Ni-22Al with 10, 20, and 30Pt was investigated in terms of oxidation kinetics, scale evolution and resulting composition profiles during heating to 1150°C in air. Platinum addition did not appear to affect the nature of the native oxide layer present on the γ '-based alloys at room-temperature; however, it was found that the presence of increasing Pt content aided in promoting the establishment of a continuous Al2O3 scale during heating the γ '-based alloys through to about 700°C. This beneficial effect can be primarily ascribed to the fact that Pt is non-reactive and its addition decreases the chemical activity of aluminum in γ '. Related to the latter, Pt partitions almost solely to the Ni sites in the ordered L12 crystal structure of γ ', which has the effect of increasing the Al:Ni atom fraction on a given crystallographic plane containing both Al and Ni. Such an effective Al enrichment at the γ ' surface would kinetically favor the formation of Al2O3 relative to NiO. A further contributing factor is that the Pt-containing γ '-based alloys showed subsurface Pt enrichment during the very early stages of oxidation. This enrichment would reduce Ni availability and increase the Al supply to the evolving scale, thus kinetically favoring Al2O3 formation.
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Authors: Takumi Nishimoto, Shigenari Hayashi, Toshio Narita
Abstract: The effects of coatings on the creep and oxidation behavior of Ti-50Al alloy were investigated at 1173K in air at a constant loading of 30MPa. The coating was formed by a two-step Cr/Al diffusion treatment and consisted of an outermost TiAl2 layer, an outer Al-rich γ layer, an intermediate γ, Laves and β mixture layer, and a Cr diffusion zone. Creep tests were also carried out with sole Cr or Al coated TiAl and also of uncoated TiAl. The oxide scales formed on the uncoated TiAl and the sole Cr coated specimens were a mixture of TiO2 and Al2O3, which displayed several exfoliations. Both the two-step Cr/Al coated TiAl and the sole Al coated specimens formed a protective Al2O3 layer and little oxide exfoliation was observed here. Significant cracks were observed in the sole Al coated TiAl, while no cracks were observed in the sole Cr coated TiAl; the two-step Cr/Al coated TiAl showed a number of cracks in the coatings. Low creep rates in the two-step Cr/Al coated TiAl could be due to the Laves phase with a hexagonal C14 structure in the intermediate, γ, β and Laves phase mixture, and the high creep rates of the sole Cr coated TiAl may originate in the major β phase component with a B2 structure in the γ, β, and Laves phase mixture.
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Authors: Yoshimitsu Shibata, Shigenari Hayashi, Toshio Narita
Abstract: A coating with duplex structure of a outer β-NiAl and an inner α-Cr layer, was formed on a Ni-40Cr-3Re (in at%) alloy with or without Zr addition, and the coated alloys were oxidized under thermal cycling in air for up to 2300ks. The coated alloys containing Zr showed a two-step parabolic oxidation, the kp1st in the early stage of oxidation was 2.6~5.4×10-11 kg2 m-4 s-1 for four alloys tested, and kp 2nd for the longer oxidation increased with increasing Zr content from 2.6~5.4×10-11 for the alloy with 0.1at%Zr to 9.6×10-11 kg2  m-4 s-1 for the alloy with 1.0at%Zr. The rapid oxidation for the alloy with 1.0at%Zr is due to the formation of ZrO2 as an internal oxide. The oxide scale in the 1st stage consisted of both α- and θ- Al2O3 with whiskers, and with further oxidation the α-Al2O3 became the major product in the 2nd stage. After the oxidation for 2300ks the as-prepared, outer β-NiAl was changed into a mixture of β-NiAl and γ’-Ni3Al for the Ni-40Cr-3Re alloy containing Zr, while in the coated Ni-40Cr-3Re alloy the outer layer became a mixture of γ’-Ni3Al and γ-Ni(Al,Cr). It was concluded that the addition of Zr into the coated Ni-40Cr-3Re alloy helps maintain high Al contents in the outer Ni-aluminide layer by forming a protective Al2O3 layer.
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Authors: Mitsunari Auchi, Shigenari Hayashi, Toshio Narita, Shigeharu Ukai
Abstract: High temperature cyclic oxidation behavior of γ'-base Ni-25Al-10Pt (in at.%) alloy was investigated at 1000°C in air with and without 30vol.%H2O. The oxidation mass gain during the initial stage of oxidation was similar in both atmospheres, but the oxidation rate in air+H2O was lower in the longer steady-state oxidation stage. Metastable Al2O3, which formed during the initial stage of oxidation, transformed completely after about 100hr of oxidation in dry air. The transformation to α-Al2O3 also occurred in air+H2O, but complete transformation to α-Al2O3 was not observed during the oxidation time in the present study. θ-Al2O3 grains remained for longer on the α-Al2O3 layer in air+H2O and became significantly coarser with oxidation time. The present results indicate that water vapor delays the metastable to α-Al2O3 phase transformation, and decreases the growth rate of α-Al2O3.
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Authors: Michihisa Fukumoto, Tsuyoshi Yokota, Motoi Hara, Toshio Narita
Abstract: A Ni aluminide layer containing Zr or Hf was formed on a Ni specimen by the simultaneous electrodeposition of Al and Zr or Al and Hf using a molten-salt bath. When the simultaneous electrodeposition of Al and Zr was carried out using molten NaCl-KCl containing 3.5 mol%AlF3 and 0.05 mol%ZrF4, the electrodeposited layers were formed in the order of Ni2Al3, NiAl3 and Al from the Ni substrate side. The ZrAl3 particles were uniformly formed in the surface region of the NiAl3 and Al layers. On the other hand, when the simultaneous electrodeposition of Al and Hf was carried out using molten NaCl-KCl containing 3.5 mol%AlF3 and 0.05 mol%HfF4, the electrodeposited layer consisted of Ni2Al3 as the inner layer and NiAl3 as the outer layer were formed with HfAl3 particles uniformly formed in the surface region of the NiAl3 layer. For the sample treated with the simultaneous electrodeposition of Al and Zr, no significant change in the mass gain was observed during the cyclic-oxidation test at 1423 K, suggesting that the sample had a high cyclic-oxidation resistance. Similarly, the sample treated by the simultaneous electrodeposition of Al and Hf had a high cyclic-oxidation resistance. An adhesive scale, having localized inward penetrations consisting of Al2O3 containing ZrO2 or HfO2, was formed on the samples having the high cyclic-oxidation resistance.
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