number of alloys can be beneficial. In this context another meaning for the term “crossover” was brought to light by Haga et al. [1250]. They studied a compositional crossover between 6xxx wrought alloys and AlSi-based casting alloys processed by high speed twin roll casting. This involved a true compositional blend resulting from mixed scrap streams rather than an overlap in material properties. Similar research was conducted on a crossover of 5xxx wrought alloys and AlSi-based casting [1251]. The alloy 5182 was contaminated with up to 2 wt% of Si and processed by vertical high-speed twin-roll casting. The final cold-rolled and annealed sheets showed promising properties, with a limiting draw ratio of 1.8 and elongation above 20% at 2 wt% of Si. Haga et al. [1251] concluded that the alloys could be used for die casting and sheet forming – evoking multipurpose alloys.

Finally, it should be mentioned that the crossover concept is also being applied in new processing routes such as additive manufacturing [1252]. In this area in particular, but also in general, we see that composition classifications that have been common for decades are beginning to break down, leaving plenty of room for alloy development.

## 9. Conclusions, outlook and future research

This article has reviewed the state of the art and the scientific challenges involved in making aluminum alloys more sustainable through transitioning to a more circular system of material recovery and reuse. It was motivated by the huge discrepancies between primary synthesis and secondary synthesis (i.e. recycling) in terms of energy consumption, GHG emissions and environmental pollution associated with mining and by-product management. The energy needed to melt aluminum scrap is 5% of that needed to reduce ore, a difference which – where exploited – translates into reduced CO₂ emissions. The amount of available aluminum scrap is also estimated to double by 2050, which indicates the urgency of this topic.

The key challenge here is the large-scale intrusion and accumulation of impurity elements in alloys, in terms of both the number of different elements and their concentrations. Here two main tasks emerge. One is to develop mature engineering alloys which are more scrap-compatible, i.e. more tolerant of certain tramp elements that intrude from scrap so as to make them more robust under conditions of both higher impurity content and higher composition variability. This would render alloys fit for the maximised use of scrap. The other task is to reduce both the number of alloys and their chemical complexity and, wherever possible, achieve consistent properties by replacing composition tuning by microstructure tuning.

These two tasks comprise research directions that address an overall future need: to establish a “science of dirty alloys” which encompasses a set of approaches that will equip aluminum alloys with higher impurity tolerance [3].

The article has reviewed and evaluated the metallurgical mechanisms behind the topics involved, including such things as the influence of scrap-related contaminants on the thermodynamics and kinetics of precipitation reactions, plus their mechanical and electrochemical effects; precipitation-free zones around grain boundaries; casting microstructures; and adjustment of processing parameters, plus the resulting mechanical, functional and chemical properties.

In the second section a few guiding questions were formulated, to which we now return. With regard to both controlling potential negative effects and realizing great benefits, what main factors require our attention?

(i) What effects do contaminants have?

<figure><img src="image_85.png" /><figcaption>**Fig. 83.** Schematic illustration of the proposed precipitation sequence by Cao et al. [1241] for alloy AlMg5.2Zn2.0Cu0.45 (in wt.%) upon aging at 180 °C with (a) and without (b) prior pre-aging (80 °C/12 h). Reprinted with permission from [1241].</figcaption></figure>
Due to their usually low solubility, most impurity elements promote the formation of intermetallic phases. These phases can affect castability, ductility, fracture toughness, fatigue, various forming limits, surface finish, corrosion, age-hardening capability and precipitation free zones. The associated effects can be positive (e.g. by controlling recrystallization during homogenization, or refining grain size during casting) or negative (e.g. for fracture properties if the particle size, shape and distribution is not well controlled). Well known in this respect is Fe, which can cause morphologically unfavorable intermetallic phases to form in many alloys. However, the nature and properties of the phases formed are highly dependent on processing and constitution, and there are many possibilities for optimization. In addition to forming intermetallics, impurity elements can also significantly modify existing intermetallics (through changes in intermetallic type or shape). A well-known example is the addition of Mn to FeSi-containing intermetallics. Here Mn can change the shape, which is very beneficial. Another effect of impurities can be segregation at interfaces, weakening mechanical properties or corrosion properties (e.g. Cu at grain boundaries). In addition to the formation of intermetallic phases, elements in the solid solution can also have effects, e.g. on the precipitation kinetics. Knowing more about how impurity elements might be used in such areas would be a useful aim in the science of dirty alloys. Another important impact of impurity elements is on the precipitation process itself, either directly through effects on phase selection and the trajectory of metastable and stable phases that form, or indirectly through interactions with vacancies that subsequently affect precipitation.

(ii) Are thermodynamic and kinetic databases sufficiently detailed and reliable as foundations for the development of “dirty alloys”, in particular in the areas of spinodal, metastable and intermetallic phases and contaminant effects on vacancies?

Detailed thermodynamic information about some of the relevant impurity elements, and specifically their interactions with the base alloy composition, is sparse when it comes to the prediction (and avoidance) of their occurrence and associated intermediate states. This is true not only for the underlying Gibbs free energy or Landau potential landscape curves, but also for the mobility coefficients, their effects on vacancies, and the nucleation barriers or respective spinodal decomposition windows.

Much more development work is required in the future on free energy descriptions of intermetallics as a function of different scrap alloying element additions. The pending questions here are: how is the competition between different intermetallics affected by impurity addition? What scrap elements are soluble in the various intermetallics? How do scrap additions modify the shapes of intermetallics?

The effect of vacancy binding due to impurity elements and the subsequent effect on diffusion and precipitation needs more investigation. Excess vacancy content during precipitation is non-constant due to such effects. Phenomena such as the “vacancy pump” have been proposed to explain some of the unusual time dependence of diffusion-controlled processes in Al-alloys (such as the logarithmic time dependence of resistivity changes). It is clear that mass transport under conditions of vacancy trapping and binding requires much work. This strongly influences the kinetics of precipitation in aluminum alloys.

(iii) Can scrap-related contaminants get trapped at lattice defects and inside precipitates? Could such trapping be used to render them harmless? Which types of thermal treatment should be applied to this end? Are all contaminant-related phases that form harmful, or are there beneficial features associated with any of the tramp elements?

Impurities are often found to become enriched in dispersoids, in intermetallics, in the bulk and at grain boundaries. Investigations are thus needed to detail which of these nano-alloying elements are harmless and which are not, e.g. in terms of embrittlement, precipitation-free zones, age-hardening kinetics, hydrogen embrittlement and/or micro-galvanic corrosion. In some well-studied scrap-related intermetallic precipitates, modest alloy modifications can be a suitable pathway for mitigating harmful effects from such precipitation states.

Some impurity elements can be deployed to segregate to precipitate interfaces and beneficially affect thermal stability; this has been done in Al-Cu based alloys. More work in this direction is required. Some tramp elements can be bad, however, and finding ways to immobilise them at trapped sites is worth considering. Can reservoirs be built into the alloy design to trap detrimental species so that

<figure><img src="image_86.png" /><figcaption>**Fig. 84.** Demonstration of the potential of an 5182 base alloy (denoted as AlMg) with the addition of 3.5 wt% Zn (denoted as AlMgZn) and 3.5 wt% Zn and 0.5 wt% Cu (denoted as AlMgZnCu). Data after pre-aging (typical forming condition) and after a paint-bake treatment (typical application condition) are shown. The forming properties deducible from the tensile tests (elongation, strain hardening) are comparable to 5182 for the alloys with added Zn and Zn + Cu. The strength after a paint-bake treatment is superior. A comparison with a common automotive 6xxx alloy for automotive applications is also shown. Reprinted with permission from [1239].</figcaption></figure>
they cannot damage other processes?

(iv) How impurity-tolerant can we make green near-commercial Al-alloys, and which contaminants are most relevant? What upper limits apply to contaminants in near-engineering Al-alloys?

The most important contaminants are Fe, Mn, Cr, Cu and Si, depending on the alloy class and the product application targeted. It was shown that with regard to some of these scrap-related contaminants, alloy tolerance can already be increased in existing alloys without any substantial loss of properties. It is important to understand that through advanced casting processes and higher quench rates, higher levels of impurities (e.g. Fe) might be made possible. Most work concerns alloys for automotive applications (5xxx, 6xxx series alloys and casting alloys), but increased impurity levels are also being discussed in the context of aircraft alloys. In general there is much scope for research into improving the impurity tolerance of established alloys, either through processing or through minor compositional measures (e.g. modification of deleterious intermetallic phases).

(v) Which crossover alloys are the most promising for combining beneficial mechanisms across established alloy families?

Such broad-band, multi-purpose alloys must be designed as universal and not as niche alloys. They should be broad in their composition tolerance and application range. This field is relatively new, but there have already been attempts to combine excellent forming properties and high strength in new AlMgZn(Cu) alloys in order to cover more automotive applications with one alloy [48,1006]. Attempts are also being made to extend the properties of existing wrought (6xxx) and cast alloys (AlSiMg) within one compositional range to broaden their applicability. Although the overall concept of such crossover alloys is very appealing, it must be considered that most of the Al produced thus far is still in use, and that the accumulation of Al out there falls into composition ranges that are roughly defined by the existing classes. Making those existing classes more robust in the face of impurities would probably be of greater benefit to the field because it would encompass the Al already in use.

(vi) What combinatorial high-throughput methods are suitable for revealing scrap-related composition-microstructure-kinetics-property trends and ranges? How can we probe damage-tolerance in the associated experiments?

Recent work suggests that the combinatorial screening of alloys for effects associated with scrap-related impurities requires the use of at least mm-thick sample sizes which can be cast, homogenised and quenched-in under conditions that approximate macroscopic processing conditions, at least roughly. Thin film combinatorial methods, or compositional alloy gradients produced by additive manufacturing or related methods which utilise rapid quenching, create microstructures that are not really comparable to those observed under real manufacturing conditions.

(vii) For which phases is it necessary to use atomistic simulation methods to understand phase (meta-) stability, impurity trapping, sublattice occupancy and phase stoichiometry ranges? In general, are there sufficiently suitable modeling techniques available by which we can analyse the effects of tramp elements on aluminum alloys?

Few reliable thermodynamic data are available on phases with > 4 components. When such phases become important in the context of contaminants from scrap, it may be expedient to study their exact composition and structure by electron microscopy and atom probe tomography and to use the results for thermodynamic calculations. If only a small fraction of tramp elements enters dispersoids or transient phases, ab initio calculations become challenging because they need a certain minimum stoichiometry to fit supercell simulations. A better thermodynamic understanding of impurity-related phases is generally important, because in some cases a suitable strategy may be to add further doping elements that render some of these intermetallic cases less harmful (i.e. Fe-containing phases become less harmful if they are doped with Mn).

(viii) How does deploying meso- and near atomic-scale characterization methods address these challenges? How can the main effects associated with tramp elements be observed and identified?

High-resolution probing techniques such as scanning transmission electron microscopy and atom probe tomography can reveal even near-ppm-range impurity effects and the associated structures of nano-precipitates. Ideally these techniques are applied to the same portion of the material in question, a technique that is referred to as correlated microscopy. Corresponding additional information on size distributions, which gives such studies statistical relevance, can be obtained using advanced synchrotron methods. In some cases, it may be necessary to conduct these studies together with ab initio calculations. A remaining weakness lies in analyzing the interaction between impurity elements and vacancies, an effect which can be particularly important in aluminum alloys.

(ix) Can supervised, knowledge-informed machine learning identify suitable nanostructure-composition-processing-property relations for the field of sustainability alloy design?

The currently most promising, valuable application of artificial intelligence methods in this area is in scrap separation and sorting, mainly applied in LIBS analysis. Future benefits for recycling and the related alloys may also come from exploiting the massive amounts of processing data provided today by the many sensors that exist in current processing lines – data gathered over many processing steps and analysed in dependence on chemical composition variations. Here, discovering trends with the help of machine learning may be a very fruitful way to use scrap in aluminum alloys efficiently in future, and also to screen composition-property relationships for scrap-compatible alloy design [1253,1254].

(x) How do processes have to be adjusted to deal with the effects of contaminant elements?

Besides improved scrap sorting, techniques for advanced casting techniques including flow optimization and more rapid cooling are gaining momentum. For instance, high solidification rates in near-net-shape casting lead to reduced through-thickness compositional gradients, higher dispersion of contaminant-affected precipitates, reduced Scheil segregation profiles, and smaller grain and dendrite sizes, and thus generate greater homogeneity in the cast material overall. The extreme case here is additive manufacturing, where high solidification rates allow the use of high concentrations of typical impurity elements (e.g. Fe) to further improve the property portfolio. Later procedures in the process chain such as heat treatments may also require adjustment (e.g. advanced homogenization for fragmentation of intermetallic phases).

It is also worthwhile in general to consider being less reliant on thermally induced precipitation to make high-strength aluminum
alloys. The reason these alloys are so sensitive to compositional variation is because the thermally induced precipitation process is also very sensitive to composition. What if we did not need to use thermally induced precipitation but could instead force the decomposition of the solid solution by external means? We could, instead, consider forcing precipitation via a “driven system”. One example of such external forcing is seen in the recently published approach of deploying cyclic plasticity to continually inject vacancies into the material to drive the decomposition of the solid solution by dynamic precipitation at room temperature [85]. This approach is very effective and much less sensitive to impurity effects. While industrializing such new processes is a challenge, they should definitely be considered in making alloys more composition-robust. High-powered ultrasonics or forms of irradiation might be interesting sources for such excitation. These and other different approaches to processing may completely change precipitation sensitivity to impurities [296,935].

(xi) What measures and approaches promise to be the most effective in improving the sustainability of secondary synthesis?

In processing, a significant impact is to be expected from scrap avoidance, streamlined scrap collection and improved scrap sorting, including the associated producer and downstream manufacturer workflows. These things will clearly have the greatest effects. The origin of scrap also matters: when expressed as global warming potential (GWP, in kgCO₂eq per metric ton), primary smelters where the material is synthesized from ores have a GWP footprint of 12.2, production from old (post-consumer) scrap have a GWP footprint of only 1.4, and production from new (in-production) scrap have a GWP footprint as low as 0.4. Further effects come from replacing all fuels used for furnace heating with renewable electrical and/or green hydrogen sources. Generally, electrification of processes should have high priority. In casting, rolling and heat treatment efforts should be directed at enhancing the dispersion of dispersoids and precipitates, including intermetallic particles that can occur when a higher impurity content enters the alloys. Incentives for establishing some of these measures might be tax regulations and/or sustainability labels that make them, and improved scrap streams, visible to customers. Ideally, high market prices would result. On the metallurgical side, all measures that enhance alloy tolerance to impurity elements have a significant effect, particularly in alloys traded in large quantities. One example is the increase in the Fe content of 6xxx sheet alloys used for vehicles. For more examples see the bulk text.

In the context of all these measures it is important to calibrate metallurgical and processing adjustments to the scrap-based alloys which are the most sustainable.

From a conceptual perspective it would surely be desirable in the future to reduce the number of alloy variants on the market, and even to develop certain standards to govern which alloys should be used for certain parts so as to avoid the often-observed wide variation in alloy types used in the same product, which makes subsequent scrap separation a challenge. Also, microstructure tuning should generally be preferred over composition tuning when adjusting and developing materials for new products. Microstructure tuning requires state-of-the-art processing equipment and both knowledge-based and machine-learning-based access to the underlying processing-structure-property relationships of alloys which contain impurities. Another very promising avenue lies in developing multi-purpose and crossover alloys. These could generally help to reduce the number of alloy variants on the market.

Product design will also have to be adjusted on the customer side where sustainable alloys made from scrap are involved. In the future, customers who use alloys with a high recycling content will more frequently have to adjust downstream processing instead of sticking to established operations. It follows that their awareness of the issues which arise when they use alloys made from scrap needs to be improved. In any case, the best results of all will generally be achieved by improving scrap separation and establishing closed producer-customer scrap cycles.

## Author contributions

Dierk Raabe, Stefan Pogatscher, Helmut Antrekowitsch, Christopher Hutchinson und Peter J. Uggowitzer designed the article's concept.

Content dealing with scrap-based aluminum alloys was contributed mainly by Dierk Raabe, Stefan Pogatscher and Chad W. Sinclair, and was revised by all other authors.

The discussion of the sustainability of aluminum alloys was conceptually designed by Dierk Raabe, Stefan Pogatscher, Helmut Antrekowitsch, Peter J. Uggowitzer and Chad W. Sinclair and was revised by all other authors.

The sections dealing with scrap-related production steps and their sensitivity to tramp elements, types and flows of aluminum scrap, secondary synthesis, recycling rates and their consequences for alloys, advanced aluminum scrap sorting, pre-treatment methods, process technology and plant technology were authored mainly by Helmut Antrekowitsch, Stefan Pogatscher and Dierk Raabe and were revised by all other authors.

The sections on near-net-shape, thin-strip, belt and chain conveyor casting methods were contributed mainly by Dierk Raabe, Stefan Pogatscher and Mario Paolantonio.

The sections on sheet-forming challenges for scrap-contaminated alloys were authored mainly by Christopher Hutchinson, Dierk Raabe, Stefan Pogatscher, Peter J. Uggowitzer, Chunhui Liu and Zhiming Li.

The section on joining scrap-contaminated alloys was authored by Philip Prangnell and Joseph Robson.

The sections on thermodynamics simulation tools for the study of scrap-related impurities and intermetallic phases and simulation methods for the study of scrap-related impurity effects on precipitation kinetics and microstructure evolution were authored mainly by Chunhui Liu, Zhiming Li, Chad W. Sinclair, Mario Paolantonio, Christopher Hutchinson, Pratheek Shanthraj, Samad Vakili, Philip Prangnell and Ernst Kozeschnik.

The section on combinatorial metallurgical methods for studying the effects of tramp elements was developed and written by Alexis Deschamps, Mario Paolantonio, Dirk Ponge and Dierk Raabe.

The section on advanced analysis tools related to the highly-resolved characterization of tramp elements was written mainly by
David Seidmann, Baptiste Gault, Frédéric De Geuser, Alexis Deschamps and Laure Bourgeois.

The section on machine-learning approaches for the development of sustainable aluminum alloys was developed by Dierk Raabe and Chad Sinclair.

The sections on powder metallurgy, additive manufacturing and recycling-friendly and contaminant-tolerant near-engineering Al-alloys was written by Moritz Roscher, Stefan Pogatscher, Peter J. Uggowitzer and Dierk Raabe.

Reflections on all of these different aspects and discussions, and summarizing thoughts on a wide range of aluminum alloys, were contributed by all authors.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

C.H.L. acknowledges financial support from the National Natural Science Foundation of China (No. U2032117). Z.L. would like to acknowledge special funding from the Construction of Innovative Hunan Province of China (2019RS1001). D.N.S. acknowledges the support of the Northwestern University Center for Atom-Probe Tomography (NUCAPT). The LEAP tomograph at NUCAPT was purchased and upgraded with grants from the NSF-MRI (DMR-0420532) and ONR-DURIP (N00014-0400798, N00014-0610539, N00014-0910781, N00014-1712870) programs. NUCAPT received support from the MRSEC program (NSF DMR-1720139) at the Materials Research Center, the SHyNE Resource (NSF ECCS-2025633), and the Initiative for Sustainability and Energy (ISEN) at Northwestern University. The research on aluminum alloys was supported by the Office of Naval Research, Dr. William M. Mullins, grant officer. D.N. S. is grateful to D. Isheim for managing the atom probe tomography center at Northwestern University. P.B.P. and J.D.R. thank the EPSRC, LightForm Programme grant, (EP/R001715/1) for supporting aspects of this work. S.P. gratefully acknowledges financial support from the Austrian Federal Federal Government for Digital and Economic Affairs, the National Foundation for Research, Technology and Development and the Christian Doppler Research Association. E.K. gratefully acknowledges financial support from the Austrian Federal Government (in particular from Bundesministerium für Verkehr, Innovation und Technologie and Bundesministerium für Wissenschaft, Forschung und Wirtschaft) represented by Österreichische Forschungsförderungsgesellschaft mbH and the Styrian and the Tyrolean Provincial Government, represented by Steirische Wirtschaftsförderungsgesellschaft mbH and Standortagentur Tirol, within the framework of the COMET Funding Programme. L.B. acknowledges the use of the instruments and scientific and technical assistance at the Monash Centre for Electron Microscopy, a Node of Microscopy Australia. This research used equipment funded by Australian Research Council grant LE0454166.

Several of the authors express their sincere thanks for inspiring discussions about sustainable aluminum with companies such as AMAG, Hydro and Alcoa.

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