Directional Solidification Experiments Research Articles

Modelling freckles and spurious grain formation in directionally solidified superalloy castings

Segregation channels with misoriented spurious grains, known as freckles, are an unacceptable casting defect in superalloy turbine blades. A digital-twin method to predict segregation channels was proposed in our previous studies; however, the formation of spurious grains was ignored. Here, we extend the digital twin methodology by incorporating dendrite fragmentation, which is recognized as the predominant mechanism in the formation of spurious grains. The flow-induced fragmentation process has been refined to account for the timing of dendrite pinch-off. A three-phase mixed columnar-equiaxed solidification model was used to track the motion of the crystal fragments. Directional solidification experiments for superalloy casting were conducted in an industrial-scale Bridgman furnace, and the distribution of spurious grains in the freckles was metallographically analysed. Excellent simulation-experiment-agreement was achieved. Based on this study, the formation of spurious grains within the segregation channels is mainly caused by the flow-driven fragmentation mechanism. Experimentally measured freckles can be reproduced only if the timing of the dendrite pinch-off is considered.

Explanation for the linear solid/liquid interface recoil observed during directional solidification of a TRIS-NPG alloy under microgravity conditions

During the initial transient stage of a directional alloy solidification experiment, a solid/liquid interface asymptotically recoils from a position that is given by the liquidus temperature to a position given by the solidus temperature. Recent observations onboard the International Space Station revealed that for the organic compound TRIS-NPG, the recoil appears much larger and varies linearly with time. In addition, such conditions were found that the high-temperature non-facetted plastic phase gradually dissolves and, although it seems contradictory to the interpretation of the thermodynamics of the binary system, the low-temperature facetted phase comes into direct contact with the liquid. Both unexpected observations can be understood by assuming that the TRIS-NPG alloy gradually decomposes at the hot side of the furnace. The decomposition products are then transported to the solid/liquid interface by diffusion and the sample motion. The presence of decomposition products changes the binary alloy into a TRIS-NPG-X ternary alloy, with a liquidus temperature that decreases with an increasing amount of decomposed substances.

Solidification paths of Al-Cu-Sn alloys: Comparison of thermodynamic analyses and solidification experiments using in situ X-radiography

The increasing importance of Al-Cu-Sn alloys as materials for producing self-lubricating bearing materials in automotive industries requires the development of uniform microstructures with improved performance, which could be achieved by a precise control of solidification processes. Adding Sn to Al-Cu binary alloy could dramatically alters the solidification path, generating liquid phase separation and monotectic reaction. In this paper, Al-10 wt% Cu-X wt% Sn (with X = 0; 5; 10 and 20) alloys have their solidification paths investigated by three different complementary approaches. Firstly, the solidification paths were calculated by using the CALPHAD method through Thermo-Calc software revealing the sequence of transformations that could occur during the solidification of these alloys, from the formation of the initial α-Al dendrites to the final eutectic reaction. Secondly, experimental thermal analysis was carried out by DSC (Differential Scanning Calorimetry), which reveals the successive events that occur during the controlled melting and cooling of these alloys. Thirdly, directional solidification was performed on all alloys, with in situ and real-time observations achieved through the utilization of X-radiography. The comparison between the various approaches showed a suitable correspondence between the history of the alloy solidifications computed by Thermo-Calc and those obtained experimentally (DSC and directional solidification experiments). Additional information about the dynamics of each reaction was obtained during the directional solidification experiments in terms of microstructures, segregation, and the genesis of the liquid phase separation that occurred for high Sn-content alloys.

Microstructure and Tensile Properties of Ni-Base Superalloy IN738LC according to Solidification Rate and Heat Treatment

The strength of Ni-base superalloys mainly depends on the γ' precipitates that improve the strength of the materials at high temperatures. The presence of γ' particles within the matrix restricts dislocation movement, and optimized heat treatments can tailor the size, shape, and volume fraction of γ'. In this study the effects of solidification rate and solution temperature on the tensile properties of IN738LC superalloy were investigated. The secondary dendritic arm spacing of casting materials with different diameters was measured and the solidification rate of the casting materials was derived by comparing the results of the solidification microstructure obtained from a directional solidification experiment. The D17 material, which had a faster solidification rate, showed higher values of tensile strength and yield strength than the D60 material, which had a slower solidification rate. The study also concluded that the monomodal γ' precipitates in the S80 material have higher tensile strength and yield strength at room temperature and 760℃ than the bimodal γ' precipitates in the S20 material. As for the deformation behavior at 760℃, an isolated stacking fault was observed in the S20 material only within the large γ’ precipitates. In the S80 material, the high dislocation density increased the yield strength due to the strong interaction between dislocations and fine γ’ precipitates.

On the Effect of Interphase Boundary Energy Anisotropy on Morphologies: A New Type of Eutectic Grain Observed in a Three-Phase Eutectic System

Eutectic microstructures are dramatically affected by the anisotropy in interphase boundary energy. Depending on this anisotropy function, different eutectic grains may grow simultaneously at the same experimental conditions. In all reported quasi-isotropic and anisotropic two-phase and three-phase eutectic grains in thin samples, lamellar morphology is observed and the microstructure is essentially two dimensional (2D), since the interphase boundaries are perpendicular to the sample walls. Using the β(In)–In2Bi–γ(Sn) system and real-time solidification experiments in thin samples, we introduce a unique and new type of anisotropic three-phase eutectic grain, entitled here as “Laminated Matrix with Rods (LMR).” In this grain, due to the anisotropy in In2Bi/γ(Sn) interphase boundary, the evolving phases, and hence, the microstructures observed through the two glass plates of the thin sample are completely different, despite the strong confinement effect. During rotating directional solidification (RDS) experiments, the morphology or the aspect ratio of all phases changes periodically and drastically. Specifically, In2Bi, β(In), and γ(Sn) phases evolve from all being lamellar perpendicular to the sample walls to the matrix, elongated/trapezoidal rods, and a lamella parallel to the sample walls, respectively. Our experimental results show that these morphological transitions are due to change in the interphase boundary orientation with respect to the growth direction.Graphical abstract

Effects of shell mold heating temperature on microstructures and freckle formation of single crystal superalloys

To study the effects of shell mold heating temperature on the microstructure and freckle formation of single crystal superalloys, the directional solidification experiment and simulation were conducted with designed stepwise specimens. The temperature field and morphology of mushy zone were analyzed. The results show that the primary and secondary dendrite arm spacings both decrease with the rise of shell mold heating temperature. This reduces the permeability of the liquid in the mushy zone and the width of the thermal-solutal convection channel, which reduces the formation tendency of freckles, the width of freckles and the number of dendritic fragments in freckled areas. In addition, with the increase of shell mold heating temperature, the cooling rate of liquid in the mushy zone increases, which reduces the cooling time of the melt in the mushy zone, weakens the breaking capability of liquid flow to the dendrite, and further reduces the tendency of freckle formation in single crystal superalloy castings.

Grain growth competition and formation of grain boundaries during solidification of hcp alloys

Grain growth competition during directional solidification of a polycrystal with hexagonal (hcp) symmetry (Mg-1wt%Gd alloy) is studied by phase-field modeling, exploring the effect of the temperature gradient G on the resulting grain boundary (GB) orientation selection. Results show that selection mechanisms and scaling laws derived for cubic (fcc, bcc) crystals also apply to hcp materials (within their basal plane), provided a re-estimation of fitting parameters and re-scaling to account for the sixfold symmetry. While grain growth competition remains stochastic with rare events of unexpected elimination or side-branching along the developing GBs, we also confirm an overall transition from a geometrical limit to a favorably oriented grain limit behavior with an increase of thermal gradient within the dendritic regime, and the progressive alignment of dendrites and GBs toward the temperature gradient direction with an increase of G during the dendritic-to-cellular morphological transition. Comparisons with original thin-sample directional solidification experiments show a qualitative agreement with PF results, yet with notable discrepancies, which nonetheless can be explained based on the stochastic variability of selected GB orientations, and the statistically limited experimental sample size. Overall, our results extend the understanding of GB formation and grain growth competition during solidification of hcp materials, and the effect of thermal conditions, nonetheless concluding on the challenges of extending the current studies to three dimensions, and the need for much broader (statistically significant) data sets of GB orientation selected under well-identified solidification conditions.

The effect of confinement on thermal convection and longitudinal macrosegregation in directionally solidified dilute succinonitrile–camphor alloy

Directional solidification experiments were conducted in a succinonitrile–0.24 wt% camphor alloy with an emphasis on the planar front interface temperature dynamics using different sample thicknesses. The interface temperature was found to depend significantly on the thickness due to non-negligible convection effects in the thicker samples. The results were interpreted with the help of an order of magnitude analysis and a boundary layer model, which permitted estimation of the solute macrosegregation profile. The experiments and corresponding analyses performed in this work constitute an experimental characterization of convection effects as a function of sample thickness.

The Influences of Micro-Alloying Element Sn and Magnetic Field on the Microstructure Evolution of Al–Bi Immiscible Alloys

An investigation was conducted through directional solidification experiments to explore the impact of micro-alloying element Sn and a magnetic field on the solidification behavior of immiscible Al–Bi alloys, as well as the combined effect of Sn and the magnetic field. Experimental results show that the size distribution of the dispersed particles in the low-speed solidified Al–3.4 wt.%Bi alloy presents two peaks, while it only shows one peak when solidified at a relatively high speed. The addition of Sn not only can enhance the nucleation rate and the number density of the Bi-rich droplets in the sample, but also decrease the Marangoni migration velocity and the axial resultant velocity of minority phase droplets in front of the solidification interface. Thereby it promotes the formation of Al–Bi alloys with a well-dispersed microstructure. A static magnetic field with the strength of 0.2 T increases the number density of the dispersed particles and decreases the average size and the size distribution width of the dispersed particles. Under the effect of Sn addition and static magnetic field, the average radius of the dispersed particles R and the solidification velocity V0 satisfy R∝V0−1/3 when the alloy was solidified at a relatively low velocity, R and V0 satisfy R∝V0−1/2 when the alloy is solidified at a high velocity.

Enhancing sustainable valorization: Harmless synergistic melting treatment for high-value vitreous products from MSWI fly ash and electrolytic manganese residue

The waste-to-energy and manganese industries face significant ecological challenges due to two major risk sources: municipal solid waste incineration (MSWI) fly ash and electrolytic manganese residue (EMR), especially, the MSWI fly is classified as hazardous waste. High temperature melting is a promising method for harmless disposal of solid wastes. However, it has yet to be industrialized due to the high costs and energy consumption. This study proposes using EMR as an additive to co-melt with MSWI fly ash, aiming to develop a method that minimizes energy consumption while producing high value-added products. To this end, the phase evolution and phase-change cooling characteristics during the co-melting process of MSWI fly ash and EMR were experimentally investigated. XRD and SEM analyses revealed that pure vitreous slag can be obtained when mixtures are heated to 1500 °C for 120 min with ≥40 wt% EMR addition under natural air-cooling conditions. Additionally, to produce vitreous slag by air-cooling and increase MSWI fly ash treatment capacity, the molten mixture with 30 wt% EMR addition was adopted in the directional solidification experiments to establish a predictive model relating the average cooling rate to the glass content. The findings ultimately contribute to the advancement of melting-based industrial applications.

X-radiography front tracking gradient furnace for directional solidification of bulk Al-alloys

A unique gradient furnace for directional solidification experiments with bulk Al-alloy samples developed at German Aerospace Center is presented. It allows for in situ process control in solidifying samples by using x-radiography, and further insight into the solidification process is gained in combination with x-ray computational tomography on the solidified samples. Tracking of interfaces during directional solidification of bulk samples via in situ x-radiography (TIREX) enables the investigation of the melting process and observation of the movement of the entire mushy zone through the sample, tracing the solid–liquid interface during directional solidification and correlating the observations with the microstructure of the samples. Monitoring the temperature profile inside the sample by in situ observation of the length of the mushy zone is particularly important because the temperature gradient G and the rate of interfacial growth v determine the microstructure of solidification. The x-radiography setup offers temporal and spatial resolutions of 0.5 s and 70 μm, respectively, with a field of view of 10 × 50 mm2. Constant solidification velocities of up to 0.15 mm s−1 at a temperature gradient of up to 8 K mm−1 can be achieved in a temperature range of 537–1373 K. A flat solid–liquid interface inside a rod-like sample with 5 mm diameter is achieved by surrounding the sample by thermal isolating graphite foam. Performance tests with hypoeutectic Al–10 wt. % Cu alloy samples show the functionality of the furnace facility.

Directionally solidified structure of peritectic steel

ABSTRACT The solidification structure of peritectic steels (15CrMo and 20CrMo) was studied using directional solidification experiments. An island dendrite structure was observed in the hypoperitectic steel (15CrMo) at growth velocities of 15, 50, and 80 μm·s−1. While a traditional peritectic dendritic structure was observed in the hyperperitectic steel (20CrMo) at growth velocities of 15 and 50 μm·s−1, an island dendrite structure was observed at a growth velocity of 80 μm·s−1. An analysis of the solute distributions near the liquid-solid interface during solidification revealed the role of the steel grade and cooling velocity on the formation of island dendrite structures. Higher cooling velocities caused higher carbon concentration gradients in the liquid phase near the liquid-solid interface, leading to a stronger driving force for the peritectic reaction and, consequently, a more favourable formation of island dendrite structures. Hypoperitectic steel is more prone to the formation of island dendrite structures than hyperperitectic steel.

Preliminary system for data assimilation to infer material parameters from directional solidification experiments: twin experimental study using phase-field method

The integration of phase-field (PF) simulations and in situ observations is a promising approach for understanding dendrite growth. In this study, a preliminary data assimilation system is developed to integrate PF simulations and in situ real-time X-ray radiography during the directional solidification of a binary alloy. In this system, only the region around the tip of a primary arm is used for data assimilation. The validity of the developed system is confirmed through twin experiments for columnar dendrite growth with different inclined angles of preferred growth direction.

Investigation of Al-20Sn-10Cu alloy directional solidification by laboratory X-radiography

Al-based alloys with a soft phase such as Sn are extensively used for bearing components due to their self-lubricating properties. Al-Sn alloys lack the ability to support heavy loads so the alloying with Cu as a third element provides solution strengthening of the aluminium matrix. A crucial issue in the manufacturing of Al-Sn-Cu alloys is the miscibility gap in the phase diagram of the system. Liquid immiscibility is responsible for severe segregation during the solidification process, due to the large density difference between the Al-rich and Sn-rich liquids, which limits their utilization in industry. It is therefore both scientifically and technically important to accurately understand their solidification path. In the present work, the solidification of a ternary Al-20wt.%Sn-10wt.%Cu alloys was investigated in-situ by using X-radiography. Directional solidification experiments were performed on sheet-like samples in the laboratory device SFINX (Solidification Furnace with IN-situ X-radiography), which consists of a Bridgman-type gradient furnace and an X-radiography system. The solidification sequence was determined based on the observation of the recorded images, enlightening the successive steps of the solidification path. These observations were compared to predictions obtained from thermodynamic calculations. Complementary post-mortem microscopic analyses showed that the dendrite primary trunk and secondary arms developed along <110> crystallographic axes instead of the usually expected <100>.

Competitive growth during directional solidification experiments of 〈1 1 1〉 Dendrites

Competitive growth is a key topic in directional solidification, however, to the authors' best knowledge, there are no experimental or numerical studies on competitive growth between neighbouring 〈111〉 dendrites. The secondary arms of 〈111〉 dendrites can grow with more favourable orientation than those of 〈100〉 dendrites and this has implications for the competitive growth mechanism. An experimental apparatus was developed for in-situ directional solidification with a transparent model alloy, Neopentyl Glycol-35 wt% (D)Camphor (NPG-35wt.%DC), which has 〈111〉 dendrite orientation. Seven tests were conducted with different temperature gradients and isotherm speeds to investigate competitive growth behaviour. Multiple grains were identified in each test with examples of competition at converging and diverging grain boundaries as well as obedience and disobedience with the well-known Walton-Chalmers rule. Unfavourably oriented crystal colonies at diverging grain boundaries were able to outgrow favourably oriented colonies via tertiary branching. Overgrowth by the unfavourably oriented crystal was linked to the advantageous growth directions of secondary arms in 〈111〉 dendrites. Automated dendrite tip velocity tracking further elucidated the tertiary branching mechanism that allowed the unfavourably oriented crystal colonies to stabilise along the growth direction. It is proposed that the deviation from the Walton-Chalmers rule of competitive growth is probabilistic and depends on the initial seeding as well as the 3D nature of the experiments.

Constitutional supercooling and corresponding microstructure transition triggered by high magnetic field gradient during directional solidification of Al-Fe eutectic alloy

Directional solidification experiments of eutectic AlFe alloys were carried out under different high magnetic field gradients. High magnetic field gradient changed the microstructure selection during solidification process, induced the solidification microstructure to undergo eutectic instability, cellular transition, single-phase instability, and dendrite transition, which is similar to the planar-cellular-dendritic crystal growth pattern transition usually induced by an increasing growth velocity without magnetic field. The single phase was proved to be formed through an independent nucleation mechanism during single-phase instability. The effect of high magnetic field gradient on solidification was analyzed. Through the coupling effect of magnetic force and Lorentz force on solute migration and diffusion during solidification, high magnetic field gradient triggered a constitutional supercooling at the front of solid-liquid interface, which led to the growth pattern transition. A solidification model of eutectic alloy under high magnetic field gradient was proposed, and the microstructure selection map of AlFe alloy under gradient magnetic field was qualitatively drawn for the first time. This work proved that an alloy material with a microstructure usually obtained at high growth velocity can be obtained at a low growth velocity by applying a high magnetic field gradient, and suggested a new potential method for the future controlling of alloy structures and properties.

Concurrent model for sharp and progressive columnar to equiaxed transitions validated by directional solidification experiments processed in microgravity conditions

Columnar and equiaxed structures, which occur during solidification of metallic alloys, influence the texture and properties of castings, welded joints and additively manufactured components. During transient solidification, where grain refiner particles provide the predominant nucleation mechanism, a Columnar to Equiaxed Transition (CET) occurs when conditions that had originally favoured directional columnar growth change to those favouring equiaxed. Constitutional undercooling ahead of the columnar front can permit equiaxed nucleation and growth. By carrying out experiments in microgravity conditions, liquid flows due to thermal and solutal buoyancy effects are suppressed. In these diffusion-controlled conditions, we have observed examples of both sharp (clear) and progressive (gradual) CET. The experimental outcomes, especially the observation of a progressive CET, has highlighted the need for a continuum model that allows for competitive columnar and equiaxed structure development; hence, the Concurrent Columnar to Equiaxed Transition (C2ET) model is proposed. The C2ET is thermally transient and relies on the well-known concept of extended growth for impingement mechanics; thereby, greatly reducing numerical complexity. Importantly, the proposed approach removes the need for a specific equiaxed-blocking criterion, which is often proposed as an essential requirement in other CET models. The C2ET model is validated by four experimental solidification scenarios: two velocity jumps and two thermal-gradient decreases. The velocity jumps induced sharp CETs; whereas, thermal-gradient decreases gave progressive CETs. The C2ET model gave good agreement for the columnar and equiaxed transition zones for both sharp and progressive CET. Results are compared with the classic Hunt model. Unlike Hunt’s model, the C2ET model predicted all macrostructure transitions faithfully using a single (or consistent) set of nucleation input parameters across all four scenarios. Since, the same level of grain refinement was used in each experiment, a consistent set of nucleation parameters was expected. The validated approach can enable effective simulation at lower computational cost for industrial processes that rely on a solidification processing step.

Equiaxed grain structure formation during directional solidification of a refined Al-20wt.%Cu alloy: In situ analysis of temperature gradient effects

Three series of directional solidification experiments on refined Al-20wt.%Cu alloys have been carried out with different temperature gradients, and for each of them a wide range of cooling rates were applied. The experiments were performed in horizontal configuration to minimize the impact of gravity-driven phenomena and characterized in situ and in real-time by using the X-radiography technique. The influence of the temperature gradient on the microstructure formation (impact of Temperature Gradient Zone Melting: TGZM), the nucleation distance, the average grain size and morphology (elongation factor and grain orientation) have been analysed quantitatively. The experimental results are discussed with current theoretical models and similar experimental works.

Peritectic equilibrium in Fe-Co alloys

Abstract Recent results of directional solidification experiments with Fe–Co alloys were not consistent with the presently accepted peritectic phase diagram. Therefore, the Fe-rich part of this phase diagram was re-examined. High-temperature gradient plane front solidification was carried out at a low velocity. After quenching of the specimen from the peritectic temperature, the compositions of the phases close to the solid/liquid interface were determined through electron probe microanalysis. Using these results together with previously published phase diagram information, an improved phase diagram is proposed with the peritectic equilibrium at T p = 1774 K, C δ = 17.7, C γ = 18.1 and C L = 19.5 at.% Co.

Rotating Directional Solidification of Ternary Eutectic Microstructures in Bi-In-Sn: A Phase-Field Study.

For the first time, the experimental processing condition of a rotating directional solidification is simulated in this work, by means of a grand-potential-based phase-field model. To simulate the rotating directional solidification, a new simulation setup with a rotating temperature field is introduced. The newly developed configuration can be beneficent for a more precise study of the ongoing adjustment mechanisms during temperature gradient controlled solidification processes. Ad hoc, the solidification of the ternary eutectic system Bi-In-Sn with three distinct solid phases is studied in this paper. For this system, accurate in situ observations of both directional and rotating directional solidification experiments exist, which makes the system favorable for the investigation. The two-dimensional simulation studies are performed for both solidification processes, considering the reported 2D patterns in the steady state growth of the bulk samples. The desired phase ordering repeat unit is obtained within both simulation types. By considering anisotropy of the interfacial energies, experimentally reported tilted lamellae with respect to normal vectors of the solidification front, as well as predominant role of anisotropy in tilting phenomenon, are observed. The results are validated by using the Jackson–Hunt analysis and by comparing with the existing experimental data. The convincing agreements indicate the applicability of the introduced method.