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At least 19 records

Chemical order transitions within extended interfacial segregation zones in NbMoTaW

Interfacial segregation and chemical short-range ordering influence the behavior of grain boundaries in complex concentrated alloys. In this study, we use atomistic modeling of a NbMoTaW refractory complex concentrated alloy to provide insight into the interplay between these two phenomena. Hybrid Monte Carlo and molecular dynamics simulations are performed on columnar grain models to identify equilibrium grain boundary structures. Here our results reveal extended near-boundary segregation zones that are much larger than traditional segregation regions, which also exhibit chemical patterning that bridges the interfacial and grain interior regions. Furthermore, structural transitions pertaining to an A2-to-B2 transformation are observed within these extended segregation zones. Both grain size and temperature are found to significantly alter the widths of these regions. An analysis of chemical short-range order indicates that not all pairwise elemental interactions are affected by the presence of a grain boundary equally, as only a subset of elemental clustering types are more likely to reside near certain boundaries. The results emphasize the increased chemical complexity that is associated with near-boundary segregation zones and demonstrate the unique nature of interfacial segregation in complex concentrated alloys.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Understanding interfacial segregation in polymer blend films with random and mixed side chain bottlebrush copolymer additives

Bottlebrush polymers are complex macromolecules with tunable physical properties dependent on the chemistry and architecture of both the side chains and the backbone. Prior work has demonstrated that bottlebrush polymer additives can be used to control the interfacial properties of blends with linear polymers but has not specifically addressed the effects of bottlebrush side chain microstructures. Here, using a combination of experiments and self-consistent field theory (SCFT) simulations, we investigated the effects of side chain microstructures by comparing the segregation of bottlebrush additives having random copolymer side chains with bottlebrush additives having a mixture of two different homopolymer side chain chemistries. Specifically, we synthesized bottlebrush polymers with either poly(styrene-ran-methyl methacrylate) side chains or with a mixture of polystyrene (PS) and poly(methyl methacrylate) (PMMA) side chains. Furthermore, the bottlebrush additives were matched in terms of PS and PMMA compositions, and they were blended with linear PS or PMMA chains that ranged in length from shorter to longer than the bottlebrush side chains. Experiments revealed similar behaviors of the two types of bottlebrushes, with a slight preference for mixed side-chain bottlebrushes at the film surface. SCFT simulations were qualitatively consistent with experimental observations, predicting only slight differences in the segregation of bottlebrush additives driven by side chain microstructures. Specifically, these slight differences were driven by the chemistries of the bottlebrush polymer joints and side chain end-groups, which were entropically repelled and attracted to interfaces, respectively. Using SCFT, we also demonstrated that the interfacial behaviors were dominated by entropic effects with high molecular weight linear polymers, leading to enrichment of bottlebrush near interfaces. Surprisingly, the SCFT simulations showed that the chemistry of the joints connecting the bottlebrush backbones and side chains played a more significant role compared with the side chain end groups in affecting differences in surface excess of bottlebrushes with random and mixed side chains. This work provides new insights into the effects of side chain microstructure on segregation of bottlebrush polymer additives.

36 MATERIALS SCIENCE↗

Effect of microalloying additions on microstructural evolution and thermal stability in cast Al-Ni alloys

Enhancement of thermal stability in Al-Ni alloys through microalloying with slow-diffusing elements, specifically Zr, has been previously reported which is attributed to Zr segregation at the Al/Al 3 Ni interface. In this study, we explore the influence of microalloying Al-Ni alloys with Zr, Ti, V, and Fe on microstructural evolution, hardness, and electrical and thermal conductivity across a range of heat-treatment temperatures from 300 to 450 °C. The distribution of microalloying elements and precipitates after heat treatment is characterized using atom probe tomography (APT). Our investigation confirms Zr segregation to the Al/Al 3 Ni interface, while similar interfacial segregation is absent with the addition of Ti, V, and Fe. Additionally, our analysis of the Al 3 Ni microfiber morphology reveals that their coarsening and spheroidization rates are similar with and without interfacial segregation; thus, retaining the fiber reinforcement through interfacial segregation of slow diffusing elements may not be an effective strategy. Precipitation of L1 2 nanoparticles was found to be the dominant mechanism affecting enhanced hardness and electrical conductivity in Al-Ni-Zr alloys, attributed to precipitation strengthening and solute depletion, respectively. Similar precipitation was not observed for additions of Ti, V, and Fe following heat treatment. We provide a thermodynamic explanation for this limitation. Furthermore, the findings of this study suggest that an effective approach for designing Al-Ni alloys should involve prioritizing microalloying elements to maximize L1 2 precipitation and minimize solute content in the FCC-Al matrix post heat treatment, rather than focusing on Al/Al3Ni interfacial segregation.

36 MATERIALS SCIENCE↗

Segregation competition and complexion coexistence within a polycrystalline grain boundary network

Interfacial segregation can stabilize grain structures and even lead to grain boundary complexion transitions. However, understanding of the complexity of such phenomena in polycrystalline materials is limited, as most studies focus on bicrystal geometries. In this work, we investigate interfacial segregation and subsequent complexion transitions in polycrystalline Cu-Zr alloys using hybrid Monte Carlo/molecular dynamics simulations. No significant change in the grain size or structure is observed upon Zr dopant addition to a pure Cu polycrystal at moderate temperature, where grain boundary segregation is the dominant behavior. Segregation within the boundary network is inhomogeneous, with some boundaries having local concentrations that are an order of magnitude larger than the global value and others having almost no segregation, and changes to physical parameters such as boundary free volume and energy are found to correlate with dopant concentration. Further, another alloy sample is investigated at a higher temperature to probe the occurrence of widespread transitions in interfacial structure, where a significant fraction of the originally ordered boundaries transition to amorphous complexions, demonstrating the coexistence of multiple complexion types, each with their own distribution of boundary chemical composition. Overall, this work highlights that interfacial segregation and complexion structure can be diverse in a polycrystalline network. Here, the findings shown here complement existing computational and experimental studies of individual interfaces and help pave the way for unraveling the complexity of interfacial structure in realistic microstructures.

36 MATERIALS SCIENCE↗

Disconnection-Mediated Transition in Segregation Structures at Twin Boundaries

Twin boundaries play an important role in the thermodynamics, stability, and mechanical properties of nanocrystalline metals. Understanding their structure and chemistry at the atomic scale is key to guide strategies for fabricating nanocrystalline materials with improved properties. In this work, we report an unusual segregation phenomenon at gold-doped platinum twin boundaries, which is arbitrated by the presence of disconnections, a type of interfacial line defect. By using atomistic simulations, we show that disconnections containing a stacking fault can induce an unexpected transition in the interfacial-segregation structure at the atomic scale, from a bilayer, alternating-segregation structure to a trilayer, segregation-only structure. This behavior is found for faulted disconnections of varying step heights and dislocation characters. Supported by a structural analysis and the classical Langmuir–McLean segregation model, we reveal that this phenomenon is driven by a structurally induced drop of the local pressure across the faulted disconnection accompanied by an increase in the segregation volume.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of Hydrogen Annealing, Sulfur Segregation and Diffusion on the Cyclic Oxidation Resistance of Superalloys: a Review

This review is based on the phenomenon of improved oxide scale adhesion for desulfurized superalloys. The proposed adhesion mechanism involves sulfur interfacial segregation and scale-metal bond weakening. Sulfur surface segregation on superalloys is examined as a function of temperature and sulfur content and related to classical behavior predicted by the McLean isotherm. Effective desulfurization to less than 1 ppmw can be accomplished by hydrogen annealing and is governed by sulfur diffusion kinetics in nickel. Hydrogen annealing results in excellent cyclic oxidation resistance for a number of advanced superalloys. The concept of a critical sulfur content is discussed in terms of practical annealing conditions and section thicknesses.

Smialek, J. L.↗

Effects of hydrogen annealing, sulfur segregation and diffusion on the cyclic oxidation resistance of superalloys: A review

This review is based on the phenomenon of improved oxide scale adhesion for desulfurized superalloys. The proposed adhesion mechanism involves sulfur interfacial segregation and scale-metal bond weakening. Sulfur surface segregation on superalloys is examined as a function of temperature and sulfur content, and is related to the classical behavior predicted by the McLean isotherm. Effective desulfurization to less than 1 ppmw can be accomplished by hydrogen annealing and is described by sulfur diffusion kinetics in nickel. Hydrogen annealing results in excellent cyclic oxidation resistance for a number of advanced superalloys. The concept of a critical sulfur content is discussed in terms of practical annealing conditions and section thicknesses.

Smialek, J. L.↗

Sulfur and Moisture Effects on Alumina Scale and TBC Spallation

It has been well established that a few ppmw sulfur impurity may segregate to the interface of thermally grown alumina scales and the underlying substrate, resulting in bond degradation and premature spallation. This has been shown for NiAl and NiCrAl-based alloys, bare single crystal superalloys, or coated superalloys. The role of reactive elements (especially Y) has been to getter the sulfur in the bulk and preclude interfacial segregation. Pt additions are also very beneficial, however a similar thermodynamic explanation does not apply. The purpose of the present discussion is to highlight some observations of these effects on Rene'142, Rene'N5, PWA1480, and PWA1484. For PWA1480, we have mapped cyclic oxidation and spallation in terms of potential sulfur interfacial layers and found that a cumulative amount of about one monolayer is sufficient to degrade long term adhesion. Depending on substrate thickness, optimum performance occurs if sulfur is reduced below about 0.2-0.5 ppmw. This is accomplished in the laboratory by hydrogen annealing or commercially by melt-fluxing. Excellent 1150 C cyclic oxidation is thus demonstrated for desulfurized Rene'142, Rene'N5, and PWA1484. Alternatively, a series of N5 alloys provided by GE-AE have shown that as little as 15 ppmw of Y dopant was effective in providing remarkable scale adhesion. In support of a Y-S gettering mechanism, hydrogen annealing was unable to desulfurize these alloys from their initial level of 5 ppmw S. This impurity and critical doping level corresponds closely to YS or Y2S3 stoichiometry. In many cases, Y-doped alloys or alloys with marginal sulfur levels exhibit an oxidative sensitivity to the ambient humidity called Moisture-Induced Delayed Spallation (MIDS). After substantial scale growth, coupled with damage from repeated cycling, cold samples may spall after a period of time, breathing on them, or immersing them in water. While stress corrosion arguments may apply, we propose that the underlying cause is related to a hydrogen embrittlement reaction: Al alloy + 3 H2O = Al(OH)3 + 3H(+) + 3e(-). This mechanism is derived from an analogous moisture-induced hydrogen embrittlement mechanism originally shown for Ni3Al and FeAl intermetallics. Consequently, a cathodic hydrogen charging technique was used to demonstrate that electrolytic de-scaling occurs for these otherwise adherent alumina scales formed on Y-doped Rene'N5, in support of hydrogen effects. Finally, some TBC observations are discussed in light of all of the above. Plasma sprayed 8YSZ coatings, produced on PWA1484 without a bond coat, were found to survive more than 1000 1-hr cycles at 1100 C when desulfurized to below 0.1 ppmw. At higher sulfur (1.2 ppmw) levels, moisture sensitivity and delayed TBC failure, referred to as Desk Top Spallation, occurred at just 200 hr. Despite a large degree of scatter, a factor of 5 in life improvement is indicated for desulfurized samples in cyclic furnace tests, confirming the beneficial effect of low sulfur alloys on model TBC systems. (DTS and moisture effects are also observed on commercially applied PVD 7YSZ coatings on Rene'N5+Y with Pt-aluminide bond coats). These types of catastrophic failure were subverted on the model system by segmenting the substrate into a network of 0.010 high ribs, spaced in. apart, prior to plasma spraying. No failures occurred after 1000 cycles at 1150 C or after 2000 cycles at 1100 C, even after water immersion. The benefit is described in terms of elasticity models and a critical buckling stress.

Smialek, James L.↗

Effect of sulfur removal on Al2O3 scale adhesion

The effect of removing sulfur impurity on the adhesion of Al2O3 scale to NiCrAl was investigated in four experiments. It was found that removing sulfur to concentration less than 1 ppm per weight is sufficient to produce a very significant degree of alpha-Al2O3 scale adhesion to undoped NiCrAl alloys. Results of experiments show that repeated oxidation, and polishing after each oxidation cycle, of pure NiCrAl alloy lowered sulfur content from 10 to 2 ppm by weight (presumably by removing the segregated interfacial layer after each cycle); thinner samples became adherent after fewer oxidation-polishing cycles because of more limited supply of sulfur. It was found that spalling in subsequent cyclic oxidation tests was a direct function of the initial sulfur content. The transition between the adherent and nonadherent behavior was modeled in terms of sulfur flux, sulfur content, and sulfur segregation.

Smialek, James L.↗

Non-equilibrium phase distribution in an Al-SiC composite

The phase distribution in an Al-SiC composite has been investigated using high resolution analytical electron microscopy. Particular attention was focused on Al-SiC interfaces, matrix boundaries and impurity phases which would impede the easy glide of dislocations. Small crystallites of MgO were distributed singly and in clusters along Al-SiC interfaces in all specimens. Interfacial segregation and precipitation involving alloy species apparently affected precipitation in the matrix, where the distribution of phases was found to be very heterogeneous. Matrix phases also included unusually large constituent particles and dispersoids, a consequence of the composite processing methods. The relationship between the observed microstructure and the composite mechanical behavior reported by others is discussed. The heterogeneous distribution of matrix phases is expected to result in a wide variaiton in local yield stress and local work-hardening rate within the composite.

Nutt, S. R.↗

Adherent Al2O3 scales formed on undoped NiCrAl alloys

Changes in the spalling behavior of Al2O3 scales formed on an undoped NiCrAl alloy are described. Two samples of Ni-15Cr-13Al (wt pct), one a control and the other sanded, were subjected to 25 oxidation cycles. It is observed that adherent scales formed on the sanded sample; however, the control sample had speckled, spalled scales. The data reveal that the adherent scales are caused by repeated removal of surface layers after each oxidation cycle. It is determined that interfacial segregation of sulfur influences spallation and sulfur removal increases bonding. The effect of moisture on scale adhesions is investigated.

Smialek, James L.↗

Fracture-tough, corrosion-resistant bearing steels

The fundamental principles allowing design of stainless bearing steels with enhanced toughness and stress corrosion resistance has involved both investigation of basic phenomena in model alloys and evaluation of a prototype bearing steel based on a conceptual design exercise. Progress in model studies has included a scanning Auger microprobe (SAM) study of the kinetics of interfacial segregation of embrittling impurities which compete with the kinetics of alloy carbide precipitation in secondary hardening steels. These results can define minimum allowable carbide precipitation rates and/or maximum allowable free impurity contents in these ultrahigh strength steels. Characterization of the prototype bearing steel designed to combine precipitated austenite transformation toughening with secondary hardening shows good agreement between predicted and observed solution treatment response including the nature of the high temperature carbides. An approximate equilibrium constraint applied in the preliminary design calculations to maintain a high martensitic temperature proved inadequate, and the solution treated alloy remained fully austenitic down to liquid nitrogen temperature rather than transforming above 200 C. The alloy can be martensitically transformed by cryogenic deformation, and material so processed will be studied further to test predicted carbide and austenite precipitation behavior. A mechanistically-based martensitic kinetic model was developed and parameters are being evaluated from available kinetic data to allow precise control of martensitic temperatures of high alloy steels in future designs. Preliminary calculations incorporating the prototype stability results suggest that the transformation-toughened secondary-hardening martensitic-stainless design concept is still viable, but may require lowering Cr content to 9 wt. pct. and adding 0.5 to 1.0 wt. pct. Al. An alternative design approach based on strain-induced martensitic transformation during cryogenic forming, thus removing the high martensitic constraint, may permit alloy compositions offering higher fracture roughness.

Olson, Gregory B.↗

Crystal growth and fluid mechanics problems in directional solidification

Broadly speaking, our efforts have been concentrated in two aspects of directional solidification: (A) a more complete theoretical understanding of convection effects in a Bridgman apparatus; and (B) a clear understanding of scalings of various features of dendritic crystal growth in the sensitive limit of small capillary effects. For studies that fall within class A, the principal objectives are as follows: (A1) Derive analytical formulas for segregation, interfacial shape and fluid velocities in mathematically amenable asymptotic limits. (A2) Numerically verify and extend asymptotic results to other ranges of parameter space with a view to a broader physical understanding of the general trends. With respect to studies that fall within class B, the principal objectives include answering the following questions about dendritic crystal growth: (B1) Are there unsteady dendrite solutions in 2-D to the completely nonlinear time evolving equations in the small surface tension limit with only a locally steady tip region with well defined tip radius and velocity? Is anisotropy in surface tension necessary for the existence of such solutions as it is for a true steady state needle crystal? How does the size of such a local region depend on capillary effects, anisotropy and undercooling? (B2) How do the different control parameters affect the nonlinear amplification of tip noise and dendritic side branch coarsening?

Tanveer, Saleh↗

Toward Optimum Scale and TBC Adhesion on Single Crystal Superalloys

Single crystal superalloys exhibit excellent cyclic oxidation resistance if their sulfur content is reduced from typical impurity levels of approximately 5 ppmw to below 0.5 ppmw. Excellent alumina scale adhesion was documented for PWA 1480 and PWA 1484 without yttrium additions. Hydrogen annealing produced effective desulfurization of PWA 1480 to less than 0.2 ppmw and was also used to achieve controlled intermediate levels. The direct relationship between cyclic oxidation behavior and sulfur content was shown. An adhesion criterion was proposed based on the total amount of sulfur available for interfacial segregation, e.g., less than or equal to 0.2 ppmw S will maximize adhesion for a 1 mm thick sample. PWA 1484, melt desulfurized to 0.3 ppmw S, also exhibited excellent cyclic oxidation resistance and encouraging TBC lives (10 mils of 8YSZ, plasma sprayed without a bond coat) in 1100 C cyclic oxidation tests.

Smialek, James L.↗

Equilibrium solute segregation to matrix- θ' precipitate interfaces in Al-Cu alloys from first principles

Particular combinations of solute atoms segregated to the interface of the Al and θ ' - Al 2 Cu in Al-Cu alloys can help stabilize θ ' precipitates at high temperatures. Stabilization of such precipitates is determined by a combination of thermodynamics (including driving forces for coarsening and transformation and solute segregation tendencies) and kinetic effects (including solute diffusion and interfacial mobility in the presence of interfacial solute segregation). For some alloys such as recent Al-Cu-based alloys, multiple solutes segregate in significant quantities to interfaces, and solute-solute interactions at the interface are important, with multiple types of solutes competing for similar interfacial sites. To treat this situation, we develop and apply a statistical mechanics approach to calculate the temperature-dependent equilibrium solute atoms distribution near the coherent and semicoherent interfaces between the Al matrix and the θ ' - Al 2 Cu precipitates. The developed approach is applied to the investigation of Si, Mn, and Zr segregation at the interface, as particular combinations of these elements affect the thermal stability of the θ ' precipitates. We demonstrate that because Si and Mn atoms segregate on the same semicoherent interface, the presence of Si reduces the concentration of Mn solutes at the interface. Si atoms preferably occupy the first layer of the interface and compete with Mn atoms for one type of particular sites in the layer. Mn atoms preferably occupy the second layer of the semicoherent interface, and the Mn-Mn interaction plays an important role in their distribution. Zr atoms mostly segregate on one of the two nonequivalent sites of the second layer of the coherent interface. Due to symmetry properties of the coherent interface, the calculations show that the segregation Zr of atoms to this interface will likely lead to the formation of L 1 2 ordered Al 3 Zr layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Directional solidification with heat losses

The upward directional solidification of a dilute binary alloy in a tall, thin, two-dimensional slot is considered. Heat losses from the sidewalls produce curved isotherms, interface deformations, and melt convection. An asymptotic approach is used which relates the small heat loss to the thinness of the solidification cell, and solutions are obtained for the resulting melt convection, interface deflection, and the distribution of heat and solute. The model is compared to the numerical results of Chang and Brown (1983) which exclude the effects of solute buoyancy and thermodynamic equilibrium at the interface. The radial segregation at the interface (consistent with both interface shapes and temperature fields) is computed, and it is found that the radial segregation is independent of interfacial shapes; the radial segregation cannot be calculated from only a knowledge of the interface shape.

Brattkus, K.↗

Sulfur Impurities and the Microstructure of Alumina Scales

The relationship between the microstructure of alumina scales, adhesion, and sulfur content was examined through a series of nickel alloys oxidized in 1100 to 1200 deg. C cyclic or isothermal exposures in air. In cyclic tests of undoped NiCrAl, adhesion was produced when the sulfur content was reduced, without any change in scale microstructure. Although interfacial voids were not observed in cyclic tests of NiCrAl, they were promoted by long-term isothermal exposures, by sulfur doping, and in most exposures of NiAl. Two single crystal superalloys, PWA 1480 and Rene' N5, were also tested, either in the as-received condition or after the sulfur content had been reduced to less than 1 ppmw by hydrogen annealing. The unannealed alloys always exhibited spalling to bare metal, but interfacial voids were not observed consistently. Desulfurized PWA 1480 and Rene' N5 exhibited remarkable adhesion and no voidage for either isothermal or cyclic exposures. The most consistent microstructural feature was that, for the cases where voids did form, the scale undersides exhibited corresponding areas with ridged oxide grain boundaries. Voids were not required for spallation nor were other microstructural features essential for adhesion. These observations are consistent with the model whereby scale spallation is controlled primarily by interfacial sulfur segregation and the consequent degradation of oxide-metal bonding.

Smialek, James L.↗