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Milligan, Brian K.

Publications and source records attributed to Milligan, Brian K..

Wrought Aluminum-Cerium Alloys by Shear Assisted Processing and Extrusion

Al-Ce alloys have attracted recent interest because of their high thermal stability due to the very low solubility of Ce in the Al matrix. The Al 11 Ce 3 eutectic phase gives excellent strain hardening behavior and moderate high-temperature strength in the as-cast state. However, its strengthening effect is limited by its coarse as-cast structure. Therefore, alternative manufacturing methods such as additive manufacturing or equal channel angular pressing have been applied to refine the Al 11 Ce 3 phase to good effect. However, these techniques are both expensive and time-consuming. Therefore, this study aims to use Shear Assisted Processing and Extrusion (ShAPE), an emerging solid phase processing technique that is more easily scalable than the previously mentioned methods. ShAPE can produce useful cross-sections of an Al-8Ce-4Mg alloy while refining the Al 11 Ce 3 phase to produce a higher strength material. It was found that a low temperature ShAPE process can improve the room temperature yield strength by ~60% compared to a binary Al-4Mg alloy. Additionally, the high-temperature yield strength of the Al-Ce alloys increased by 20%, with a simultaneous 15% improvement in ductility compared to the binary Al-Mg alloy. These results highlight the potential for ShAPE as a processing technique for Al-Ce alloys.

36 MATERIALS SCIENCE↗

Upcycling of Mixed Aluminum Alloy Shredder Scrap using Shear Processing

Conservation of critical materials is an increasing area of focus in the Unites States. In 2023, aluminum was added to the US Department of Energy Final Critical Materials List which has spurred public and private research into sustainable management of these resources. Additionally, efficiency in manufacturing and conservation of natural resources are growing concerns with targets to lower global carbon emissions, as primary aluminum alloy production is energy intensive, requiring 14 MWh of electricity plus 0.4 tonnes of CO2 per tonne of Al. Due to these factors, is essential that more sustainable manufacturing methods for aluminum alloys are developed going forward. To this end, much research is ongoing on the topic of more efficient utilization and recovery. However, most of this research still requires primary aluminum in the production process. Here, it will be attempted to bypass the use of primary aluminum and produce useful material recycled from 100% post-consumer scrap. Even considering recent developments in recycling of Al scrap, there is still a large amount of post-consumer scrap that is underutilized due to high impurity content, and that amount will increase significantly as more and more aluminum alloys are utilized in vehicles. This “scrap wave” is expected to cover 80% of the demand for automotive aluminum alloys by 2050 . A challenge to be addressed before the coming scrap wave can be fully utilized is that the tolerance of manufacturing techniques to impurities or off-spec alloy compositions must be increased. Particularly, in 5000-and 6000-series alloys (the most common wrought alloys in durable products), excess iron, copper, and silicon create brittle intermetallics during casting that remain in the extruded microstructure which limit the formability, ductility, and corrosion resistance of the alloy. Concerningly, many of the highest-volume post-consumer aluminum scrap streams such as automotive shredder scrap contain a mix of alloys including both wrought and cast alloys. Their compositions can vary widely depending on geography and the time of year. Because they are mixed, they often contain high content of multiple alloying elements such as Si and Cu in higher concentrations than are found in typical wrought alloys. They may also be contaminated with non-Al alloys from fasteners that get mixed in and often have high content of unwanted elements such as Fe. As a method for utilizing these underused scrap streams that are high in tramp elements, an emerging extrusion technology is being developed at the Pacific Northwest National Laboratory (PNNL) that aims to upcycle 100% post-consumer aluminum scrap directly into extruded components without the addition of primary aluminum . This new technology, called Shear Assisted Processing and Extrusion (ShAPE), is enabling a shift away from today’s recycling paradigm by reaching deeper into lower-value scrap streams, using shredder scrap as the extrusion billet material. Sometimes referred to as Twitch or Tweak, these scrap streams result from shredding and sorting of automobiles, building materials, appliances, and consumer goods. ShAPE combines the linear axis of conventional extrusion with a rotating extrusion die. This rotating die applies large strain to the material during extrusion, which breaks up large impurity-containing intermetallic particles, reducing their deleterious effects. This has been demonstrated for 6063 machining scrap spiked with excess Fe, and Twitch scrap high in Fe, Si and Cu where strength and ductility were retained for both feedstock compositions. Additionally, the extreme plastic deformation during ShAPE enables extrusion of billets with high Si that are too brittle for processing by conventional extrusion. By using 100% post-consumer shedder scrap as feedstock, ShAPE has the potential to slash embodied energy and carbon in extruded components by >80% compared to conventional extrusion of primary aluminum alloys.

Milligan, Brian K.↗

Shear-assisted extrusion assemblies and methods

Shear-assisted extrusion assemblies are provided. The assemblies can include a billet containing assembly containing a billet comprising a billet outer material and a billet inner material in at least one cross-section; a tool operably engaged with the billet; an extrudate receiving channel configured to receive extrudate from the tool, wherein the extrudate comprises extruded outer material and extruded inner material in at least one cross-section, the extruded outer material being the same material as the billet outer material, and the extruded inner material being the same as the billet inner material. Methods for producing multi-material shear-assisted extrudate are also provided.

Komarasamy, Mageshwari↗

Feasibility Evaluation of a Solid Phase Scalable HEA Cladding Manufacturing Route

First of a kind development result on two low-energy solid-phase processes applied on an irradiation-resistant alloy, NiCoFeCrCu 0.12 , are achieved and demonstrate moderate feasibility of successful tube fabrication using shear assisted processing and extrusion (ShAPE™) and friction stir layer deposition as a bulk manufacturing process. The scope of the work is performed in four phases: 1) direct tube manufacturing of the irradiation-resistant high-entropy alloy (HEA) composite with increased strength, 2) co-shear lining manufacturing process for the increased strength and corrosion-resistant, irradiation-tolerant HEAs, 3) ShAPE of the radially gradient corrosion resistance alloy, and 4) alloy development and fabrication enabled through friction stir additive manufacturing processes among others. This report describes the development activities from April to December 2023 to manufacture a direct customizable thin-walled tubular product from irradiation-tolerant composite high-entropy alloys (C-HEAs) while the overall project is continuing in 2024.

36 MATERIALS SCIENCE↗

Cladding and Butt-Joining Dissimilar Aluminum Alloys Simultaneously via Shear Assisted Processing and Extrusion

Shear assisted processing and extrusion has been used to fabricate multi-metallic tubing that incorporates regions with clad and butt-joined structures. In this work, aluminum alloys 6061, 7075, and 1100 are combined to create a monolithic extruded tubing with weldable ends (6061), a high strength center (7075), and a corrosion-resistant cladding (1100). Optical microscopy shows a gradual, defect-free, transition between alloys at the butt-joint interfaces and a sharp transition between alloys at the clad interface. Tensile testing proved the mechanical coherency of the joint, with failure occurring outside the tri-metallic structure. In conclusion, smoothed particle hydrodynamic simulations identified a spiral pattern of the cladding alloy that leads to inconsistent cladding thickness, and identified a simplified 2-alloy combination of aluminum alloys 6082 and 2014 that accomplished the design objectives of the tri-metallic structure.

Coatings↗

Progression of creep deformation from grain boundaries to grain interior in Al-Cu-Mn-Zr alloys

Creep mechanisms are studied in θ'-Al 2 Cu-strengthened Al-Cu-Mn-Zr alloys at 300 and 350°C for (i) ACMZ, a base alloy without further alloying elements and (ii) RR350, a commercial alloy with additions of Ni and Co forming distinct grain-boundary precipitates. At high stresses, creep is dominated by dislocations bypassing θ' precipitates within grains via the Orowan mechanism, as evidenced by (i) very high stress exponent (n~20-25) and (ii) α-Al and θ' lattice strains (measured via in-situ neutron diffraction) evolving during creep in a manner consistent with load transfer from the plastically-deforming α-Al matrix to elastically-deforming θ' precipitates. At intermediate stresses, both alloys exhibit a n~3 regime, where α-Al and θ' lattice strains scale near-linearly with applied stress while remaining largely unaffected by strain accumulation, indicating that Orowan looping or dislocation pile-up around θ' is now inactive within the grains. Rather, dislocation motion occurs solely in θ'-precipitate-free zones (θ'-PFZ) where high dislocation densities are observed via TEM after creep deformation. Plastic flow at θ'-PFZ and/or localized pipe diffusion are expected to enable grain-boundary sliding (GBS), which is proposed as the rate-limiting mechanism in the n~3 regime. Ni/Co-rich precipitates at RR350 grain-boundaries, with negligible θ'-PFZ around them, share load (as determined via neutron diffraction) with the α-Al matrix more effectively than θ-Al 2 Cu precipitates at ACMZ grain-boundaries, with wide surrounding θ'-PFZ. So, high creep resistance in the n~3 GBS regime of RR350 is enabled by coarsening-resistant grain-boundary precipitates, forming without concomitant development of weak θ'-PFZ, which effectively share load with the grains.

36 MATERIALS SCIENCE↗

Solutionization via Severe Plastic Deformation: Effect on Natural Aging in an Al-Mg-Si-(Mn) Alloy

Shear Assisted Processing and Extrusion (ShAPE), a severe plastic deformation technique that is fast and scalable, was used to produce thin-wall tubing from alloy 6082 (Al-0.8Mg-0.9Si-0.7Mn) with in-situ solutionization during processing quickly followed by quenching. Quench medium and input material heat treatment were varied and natural aging behavior (T1 heat treatment) was evaluated using tensile testing. As-cast input material was found to have higher strength early in post-ShAPE natural aging and homogenized input material was found to have strengthening during natural aging. Compared to air quenching, water quenching gave greater strength both early in and after natural aging. These observations along with microscopy suggest that: 1. air quenching was too slow; 2. as-cast material was not fully solutionized but plastic deformation broke up the coarse intermetallic particles, which provided strengthening; and 3. homogenized material was solutionized well, which led to good natural aging behavior.

Milligan, Brian K.↗

Repurposing the θ (Al 2 Cu) phase to simultaneously increase the strength and ductility of an additively manufactured Al–Cu alloy

The Al–Cu–Mn–Zr (ACMZ) cast family of alloys offers unique properties and value propositions for higher strength, higher temperature lightweight components of future vehicles. Earlier research has demonstrated trade-offs in the selection of the alloy chemistry in which an increase in Cu content from 6 up to 9 wt% improves hot tear resistance but lowers ductility. However, a recent study has demonstrated that higher-Cu (9Cu) ACMZ fabricated with laser powder bed fusion additive manufacturing (AM) results in an increase in both ductility and strength when compared to as-aged microstructure of cast 9Cu alloys. The mechanisms of differing mechanical performance of the cast and AM ACMZ alloys are elucidated in the current paper through the utilization of in situ high energy x-ray diffraction (HEXRD) tensile testing wherein lattice strains of different phases are calculated and correlated to their stresses. The ACMZ alloys consisted of theta (θ) and theta prime (θ') phases (both Al 2 Cu in nominal composition) within an aluminum matrix. The larger micron-size θ phase which decorated the grain boundaries in 9Cu ACMZ cast alloys recorded small lattice strains, while the submicron, homogeneously distributed θ phase in the 9Cu ACMZ AM alloy recorded considerably higher lattice strains. The maximum stress reached in the θ phase for the cast 9Cu alloy was found to be ~280 MPa, which was lower than the AM 9Cu alloy which registered a maximum stress of ~1.4 GPa. These measurements indicate that delayed fracture of the finer intermetallic phases simultaneously improves the ductility and strength of AM 9Cu alloy relative to the cast 9Cu alloy, which exhibits early fracture of the larger intermetallic particles.

36 MATERIALS SCIENCE↗

Crystallographic orientation-dependent strain hardening in a precipitation-strengthened Al-Cu alloy

While the strengthening of Al-Cu alloys due to precipitation has been extensively studied, the effect of crystallographic orientation of the matrix and precipitates, as well as precipitate morphology, on the strain hardening behavior is not well understood. In this paper, we investigate this effect with in situ neutron diffraction during deformation of an Al-Cu alloy (206) after multiple aging treatments. Precipitate-dislocation interactions were found to change from precipitate shearing for microstructures predominantly containing GPI and θ" precipitates to Orowan looping for microstructures with primarily θ' and θ precipitates. Notably, significant anisotropy in strain hardening behavior was observed when θ' precipitates were present, which was attributed to crystallographic orientation dependent load transfer from the Al matrix to the θ' precipitates. The anisotropic load transfer is hypothesized to be caused by the extent of rotation of high aspect-ratio θ' precipitates, owing to dislocations looping around them during plastic deformation of the matrix. Predictions from an analytical model describing the anisotropic magnitude of load transfer from precipitate rotation agree well with experimental results, successfully validating the precipitate rotation hypothesis and explaining the anisotropic strain hardening behavior. This model allows for the prediction of stresses separately in the precipitate and matrix phases as a function of crystallographic orientation, only given the bulk mechanical properties.

36 MATERIALS SCIENCE↗

The synergistic role of Mn and Zr/Ti in producing θ'/L12 co-precipitates in Al-Cu alloys

Microstructural stability is a critical factor to consider when designing new alloys for high-temperature applications. An Al-Cu alloy with Mn and Zr additions has recently been developed to withstand extended exposures of up to 350 °C. The addition of Mn in combination with Zr and their segregation to precipitate interfaces play a significant role in stabilizing the metastable θ ' precipitates responsible for the alloy's hardness; however, adding Zr and Mn separately only improves the stability to 200 °C and 300 °C, respectively. To this end, the effect of the synergistic additions on interfacial structure and chemistry was studied in detail using atom probe tomography (APT) and scanning transmission electron microscopy (STEM) for Al-Cu-Mn-Zr/Ti-containing alloys subjected to long-term annealing (up to 2,100 h) in the critical temperature range, 300 °C and 350 °C, to investigate the role of Zr/Ti in increasing the θ '-precipitate stability. The APT and STEM results reveal that Mn additions stabilize θ ' long enough for the slower diffusing Zr atoms to segregate to coherent θ ' interfaces that eventually create a θ '/ L1 2 -Al 3 (Zr x ,Ti 1-x ) co-precipitate structure. The co-precipitate is highly stable, as shown by density functional theory calculations, and is a key factor that governs microstructural stability beyond 300 °C. This study reveals how solute additions with different stabilization mechanisms can work in concert to stabilize a desired microstructure, and the results provide insights that can be applied to other high-temperature alloy systems.

36 MATERIALS SCIENCE↗

Grain Refinement Effect on the Hot-Tearing Resistance of Higher-Temperature Al–Cu–Mn–Zr Alloys

The hot-tearing resistance of Al-Cu-Mn-Zr (ACMZ) alloys was investigated as a step toward introducing these new cast alloys for severe duty, higher-temperature applications, such as cylinder heads for down-sized, turbocharged automotive engines. Alloy Cu compositions were varied from 5 to 8 wt.%. Targeted Ti levels were 0.02, 0.1, and 0.2 wt.% via additions of the Al–5Ti–1B master alloy. Hot-tearing resistance was assessed by visual examination and ranking of the cracking severity in a multi-arm permanent mold casting. It was found that at high impurity contents (Fe and Si of 0.2 wt.% each), the Al–Cu–Mn–Zr alloy with 4.95 wt.% Cu exhibited the poorest hot-tearing resistance, irrespective of the grain refining amount. Microstructural analysis indicated an effective reduction in the grain size, as the Ti additions were increased to 0.02 and 0.1 wt.% Ti via the Al–Ti–B grain refiner. The finest grain size was attained with a 0.1 wt.% Ti. Based on the hot-tearing evaluation, it was found that the additional grain refining via the Al–5Ti–1B master alloy at 0.1 wt.% Ti significantly reduces the hot-tearing susceptibility at Cu contents greater than 7.3 wt.% for ACMZ alloys with low Fe and Si. These findings indicate that the best hot-tearing resistance was observed at a grain refiner level of 0.1 wt.% Ti and high Cu content (greater than 7.3 wt.%). This study to indicates that these Al–Cu–Mn–Zr alloys, which possess excellent microstructural stability and mechanical properties at elevated temperatures, can also possess excellent hot-tearing resistance.

36 MATERIALS SCIENCE↗

Impact of microstructural stability on the creep behavior of cast Al–Cu alloys

Creep behavior of three cast Al–Cu alloys at 300 °C was studied by measuring their steady state creep rates as a function of stress. Microalloying additions in two alloys stabilized the θ' (Al 2 Cu) precipitates to 300 °C, which allowed grain boundary-controlled creep deformation to dominate at low stresses in these alloys. In contrast, the instability of the microstructure at 300 °C in a conventional Al–Cu 206 alloy led to the majority of θ' precipitates transform to the θ phase. The 206 alloy displayed diminished resistance to dislocation motion and a dislocation creep mechanism dominated from the lowest stresses. A modified Coble creep model was developed to describe the experimental low-stress creep rates in the alloys with thermally stable precipitate structures. Finally, it is concluded that increasing the thermal stability of precipitates in Al–Cu alloys can provide significant improvement in their creep performance.

36 MATERIALS SCIENCE↗