Sustainable 3D Printing With Recycled Materials: A Review: Journal of Mechanical Science and Technology 37 (11) 2023
Sustainable 3D Printing With Recycled Materials: A Review: Journal of Mechanical Science and Technology 37 (11) 2023
Sustainable 3D Printing With Recycled Materials: A Review: Journal of Mechanical Science and Technology 37 (11) 2023
1007/s12206-023-1001-9
1. Introduction
Additive manufacturing (AM), or 3D printing, is an emerging prototyping and manufacturing
technique which has the capability of producing highly complex parts through layer-by-layer
addition of materials. The comparative ease of fabrication, less time from design to production
as well as lower cost, presents an advantage of 3D printing against other manufacturing tech-
niques such as machining, milling, injection and compression molding [1]. The worldwide reve-
nues of AM are expected to grow from $ 6 billion in 2016 to $ 23 billion by 2029, with there
being high demands in the aerospace, defence and medical industries [1, 2]. 3D printing en-
ables the creation of highly complex part designs that would be impractical or impossible using
traditional methods like injection molding. Unlike subtractive manufacturing processes such as
sculpting, which involve cutting through materials and generating significant waste, AM mini-
mizes material usage, resulting in reduced waste production.
This innovative technique offers numerous opportunities for sustainable and efficient material
manufacturing. Sustainability is a broad term in modern times which not only incorporates envi-
ronmental sustainability but also sustainability related to economy and society. In terms of eco-
systems, sustainability refers to the controlled use of natural resources [3]. In terms of 3D print-
ing, there can be several types of sustainability, a) using waste or post-consumer materials and
making new value-added products using them or recycling, b) using renewable feedstock ma-
terial such as biodegradable plastics including PLA. This review paper focuses on the recycled
and reused materials which are turned into 3D printing feedstock materials through different
© The Korean Society of Mechanical
Engineers and Springer-Verlag GmbH processes.
Germany, part of Springer Nature 2023 Extensive research has been carried out on the reuse and recycling of waste materials in the
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Table 1. Acronyms.
Acronyms Meanings
PLA Polylactic acid
ABS Acrylonitrile-butadiene-styrene
PET Polyethylene terephthalate
PP Polypropylene
PE Polyethylene
HDPE High density polyethylene
LDPE Low density polyethylene
TPU Thermoplastic polyurethane
FPU Furan-containing polyurethane
PU Polyurethane
AISI904L Super austenitic steel
In718 Nickel-Chromium alloy Fig. 1. Summary of the review paper.
Titanium alloy (90 % titanium, 6 % aluminium,
Ti-6Al-4V
4 % vanadium) to the environment and the planet as a whole. Fortunately, AM
AlSi10Mg
Aluminium alloy (10 % silicon, small % presents an opportunity for plastic recycling, offering a potential
magnesium and iron) alternative solution.
316L SS, 17-4PH SS Grades of stainless steel This review paper aims to provide a comprehensive review
FDM Fused deposition modeling of the various studies which show how recycled materials are
FFF Fused filament fabrication being utilized in AM technologies. There is a general trend of
SLA Stereolithography apparatus recycled materials having lower mechanical properties than the
DLP Digital light projection original materials, and the authors have tried different rein-
SLM Selective laser melting
forcements and blends to enhance the properties of the recy-
cled materials.
DMLS Direct metal laser sintering
Fig. 1 illustrates the comprehensive overview of this review
SLS Selective laser sintering
paper, while Table 1 summarizes the corresponding acronyms.
EBM Electron beam melting As depicted in Fig. 1, Sec. 2 offers a concise introduction to
DSC Differential scanning calorimetry different types of recycled materials utilized in 3D printing, high-
TGA Thermogravimetric analysis lighting the associated benefits and challenges. Sec. 3 pro-
DMA Dynamic mechanical analysis vides succinct information about the 3D printing techniques
SEM Scanning electron microscopy employed with these recycled materials. The inclusion of vari-
Dynamic covalent bonds/ ous case studies in Sec. 4 showcases the application of 3D
DCB/DEB
dynamic exchange bonds printing with recycled materials, along with any limitations en-
PSD Particle size distribution countered. Finally, Secs. 5 and 6 present the conclusions
Tg Glass transition temperature drawn from the review and outline potential areas for future
research.
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Table 3. Average cost range per kg of common materials used in 3D print- glass from old bottles and jars, papers such as cardboard and
ing (as of 2022) [66]. old newspapers, wood from furniture, and even sand. Recy-
cling these materials not only addresses the issue of waste
Material Cost range (per kg)
reduction, preventing them from being disposed of in landfills or
PLA $15-20
incinerators and causing harm to the environment, but also
ABS $20-35
contributes to the reduction of greenhouse gas emissions by
PET $20-25 minimizing the need for new material extraction through mining
PA 12 nylon $150-225 processes. From an economic perspective, recycling offers
SS Around $150 cost-saving benefits. The cost of acquiring raw materials can
Titanium, nickel alloys $350-600 be significant, whereas utilizing waste or recycled materials
significantly reduces the expenses associated with raw materi-
als, sometimes even approaching zero.
while ABS is generally obtained from petroleum. Nylon6 and While the advantages of recycling are evident, there are still
TPU are flexible materials with appropriate stiffness for 3D several challenges that require attention and resolution. One
printing [23, 25, 26]. Table 2 mentions the advantages and major challenge is the potential degradation of material proper-
disadvantages of common recycled materials and Table 3 ties after the recycling process. This issue can be addressed
presents the average cost (per kg) of common materials used by optimizing the process parameters of AM. While recycling
in 3D printing. can be achieved on a smaller scale, large-scale recycling pre-
Recycling 3D printing materials can be done in a variety of sents its own set of difficulties, with cost being a primary con-
ways, including grinding, shredding, and sieving the used ma- cern. To ensure efficiency, the cost of the recycled material
terial to be used again in future prints [26-40], or turning the should be lower than that of commercial material, while main-
material into a new product entirely [41]. Recycling can be taining properties that are superior to the recycled material.
characterized into several stages: mechanical recycling in- Further information regarding the recycling process for additive
cludes recycling the materials by traditional manufacturing manufacturing is extensively discussed in Sec. 3, providing
processes such as grinding them into pellets or powder. additional insights and details.
Chemical recycling utilizes solvents to dissolve the materials
and then reforming them through high temperatures or using
3. Sustainable production techniques
chemical processes for breaking down of polymers. Recycling
through 3D printing can provide rapid prototyping and manu- In the market, there are various AM techniques available, in-
facturing of parts with complex shapes and sizes which would cluding FDM, DLP, SLA, selective laser melting (SLM), and
be otherwise difficult to produce using traditional approaches [6, direct metal laser sintering (DMLS). FDM utilizes thermoplastic
42]. filaments for building 3D objects layer by layer. DLP and SLA
The majority of recycled materials comprise of plastics such involve the use of photopolymer resins that are cured using
as PLA, ABS, PET, HDPE, Nylon6 etc. Thermoplastics are light to create solid objects. SLM and DMLS employ metal
generally recycled using fused deposition modelling (FDM) or powders that are selectively melted or sintered using a laser,
material extrusion (MX) technique as they can be easily enabling the production of precise metal components. Each
remelted to form feedstock filament. Vat photopolymerization technique has its own merits and is suitable for different appli-
techniques such as stereolithography (SLA) and digital light cations within AM.
processing (DLP) use thermoset materials as resins which are
very difficult to recycle due to their intense cross-links. In spite 3.1 Material extrusion process
of that, there have been a number of studies on making these
thermoset materials reprocessable through dynamic covalent FDM was introduced commercially in the early 1990s by
bonds which are bonds that provide reversibility to the network. Stratasys Inc. [67]. This AM technique involves extruding ther-
In addition to plastics, there are various other materials that moplastic filaments through a heated nozzle, melting the mate-
can be recycled, including metals such as aluminum and steel, rial. Using stepper motors, the assembly moves over a platform,
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and the melted filament is deposited layer by layer, as depicted create recycled filaments. The additional details of the FDM
in Fig. 2 [2, 67]. The most commonly used thermoplastics in printing applications with these recycled materials will be dis-
commercial FDM are ABS and PLA [68]. By extruding layers of cussed in Sec. 4.
thermoplastic materials, it allows for the production of intricate
3D objects with precision and accuracy.
3.2 Vat photopolymerization
It is worth noting that the filaments used in FDM are typically
petroleum-based, which raises concerns about their environ- Photopolymerization is another AM technique wherein liquid
mental impact. polymer is cured, or solidified, using a light source. There are
During the printing process, there is a possibility of releasing predominantly two types of photopolymerization techniques.
toxic substances that can have undesirable effects on both the One of the most popular and among the earliest 3D printing
environment and health [1]. There is an ongoing commitment techniques for engineering applications is SLA which was in-
to mitigating FDM’s environmental footprint, with continuous vented in the 1980s [2, 70]. SLA uses laser as the light source
efforts focused on recycling and the exploration of sustainable in order to cure the liquid resin. The first layer of the liquid resin
materials. The efforts are underway to explore and implement solidifies as the laser beam scans the surface. This process is
alternative materials in FDM. Researchers are actively seeking repeated layer-by-layer, with the command given to the appa-
sustainable options such as biodegradable polymers, recycled ratus through a 3D drawing software, and a 3D part is formed
plastics, and renewable resources [21, 22, 25-29, 46-48, 69]. which is thermoset by nature. The resulting part has high accu-
By utilizing these eco-friendly materials, the environmental racy, high resolution and smooth surface finish. SLA allows for
footprint of FDM can be significantly reduced, ensuring a more manufacturing of complex parts with mechanical, thermal and
sustainable future for AM. optical properties comparable to thermoplastics used in stan-
To address the environmental impact, recycling strategies dard engineering and industrial applications [2, 70].
have been developed for FDM, as illustrated in Fig. 3. Recy- DLP is similar to SLA printers with the difference being the
cling filaments for FDM process can involve various materials light source. DLP printers use ultraviolet (UV) light which cures
such as plastic, paper, sand, and wood. These materials un- the entire layer simultaneously through a digital projector
dergo processes such as cutting, shredding, and grinding to screen. Hence the printing time is greatly reduced compared to
SLA [2, 71]. A schematic of SLA and DLP is shown in Fig. 4.
The resins used in SLA, DLP printers are mostly comprised
of acrylates and epoxides which are mainly obtained from fossil
resources. In order to reduce the greenhouse gas impact on
Fig. 3. Overview of the recycling strategies and materials used in filament Fig. 4. Scheme representing bottom-up and top-down vat photopolymeriza-
3D printing. tion [2].
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ABS printed material and the one made from pelletised ABS.
The average surface deviation and surface roughness of both
virgin and recycled ABS was similar. These results indicated
similar print quality between the recycled and commercial fila-
ments which was also confirmed when they successfully
printed designed engineering items, such as a nut and bolt
system and a propeller concept, using the recycled ABS mate-
Fig. 9. Young’s modulus of 3 mm printing filament with natural fibre [43]. rial. A comparison of the ultimate strength between the virgin
and recycled filaments showed that the recycled filament had
checked the mechanical performance and shrinkage for use in 13 to 49 % less ultimate strength, with the lowest percentage
3D printing so that the value of recycled PP can be improved, decrease (13 %) being that for X build orientation. There was a
and its usage can be encouraged. Composite filaments with clear decrease in the stiffness values (17 to 28 % decrease)
1.75 mm diameter/thickness were 3D printed. In this work, the with again the X build orientation having lowest percentage
tensile testing of their filaments indicated an increase in the decrease (17 %). Factors such as layer adhesion could have
strength and stiffness with higher fiber weight fraction. Both played a role in this. The failure strain showed marginal differ-
hemp and harakeke fibers showed similar reinforcing charac- ence between the recycled and commercial samples, with the
teristics, with 30 weight percent harakeke fibers showing high- samples in the z orientation showing an exception of almost
est tensile strength and young’s modulus (Figs. 8 and 9). The 50 % decrease. The authors attributed this again to the com-
printed material showed similar trend with lower values for promised layer adhesion in the recycled material. These results
strength and stiffness, which was attributed to stress relaxation indicate that there is a reduction in the mechanical properties
and void expansion during the 3D printing. The composites due to recycling of ABS, however there are issues in the manu-
containing gypsum, on the other hand, showed a different trend. facturing process, printing parameters and the sample type
For 10 weight percent gypsum, the strength was higher than which need to be resolved.
PP, which decreased with higher gypsum content. This was Mohammed et al. [44] studied the methodologies for granula-
attributed to the agglomeration of gypsum particles with higher tion of types of plastics typically found in recyclable plastic
gypsum content resulting in lower interfacial adhesion and waste and reconstituted them into FDM 3D printer filaments as
stress concentration. The stiffness was found to increase which shown in Fig. 11. The aim was also to minimize carbon foot-
was explained by reduction in polymer chain mobility. Further, print. The authors used various plastic types such as high-
the percentage shrinkage was significantly low in composites density polyethylene (HDPE) and composites of ABS with
containing 30 weight% harakeke fibers, compared to plain PP. HDPE for the filament material and the printing parameters
Another study carried out by Mohammed et al. [22] explored were optimized. Granulation was done by direct cutting through
100 % recycled ABS material for use in FDM filament as scissors and wire cutters and shredding with a paper shredder.
shown in Fig. 10. The authors obtained virgin pellet material as Sieving was then done using a 5 mm and 2.4 mm mesh sieve
well as failed/redundant 3D prints and raft/support material to separate the pieces. The filament thickness can be con-
from various sources in order to get unbiased results. The trolled by varying the temperature of the extruder. Filament with
granulation of waste ABS was performed through crushing, 1.7-1.8 mm diameter was extruded in this study. The energy
cutting and shredding (using bench vice, wire cutters and a expenditure of the printing process was investigated. They
modified paper shredder, respectively). Separation of pieces found that highly repeatable filament generation could be
was done using a mesh sieve of 5 mm. They compared the achieved, and solar power could be easily used for low carbon
print quality as well as mechanical performance of the recycled emission power. The thickness of the filament was kept within
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Fig. 12. FDM printed flower using filament made of reused PA-12 powder
[23].
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Fig. 18. Tensile strength and modulus of pure PLA, originally printed and
Fig. 17. Recycling procedure [28].
remanufactured composites specimens [52].
waste Aquafina water bottles, which were further cleaned with showed much higher tensile strength and modulus than pure
hot water and shredded with a power smart electric shredder. PLA indicating excellent reinforcement properties of continuous
The biochar was derived from packaging waste and mixed with carbon fiber (Fig. 18). The recycled carbon fiber impregnated
the shredded and dried PET in different ratios and 3D printed filament, however, did not show much improvement in tensile
(Fig. 17). XRD analysis of biochar showed well-ordered micro- properties which was expected due to the unidirectional behav-
structure of carbon due to high carbonization temperature and ior of these composites, as the carbon fiber took the load in-
a higher degree of graphitization which was also shown stead of the interfaces. The flexural strength however showed
through Raman spectroscopy. Thermogravimetric analysis better improvement than tensile strength. As the bending force
showed a 93 % residue for biochar at 700 °C indicating high was not only taken by the carbon fibers, but was also taken up
thermal stability. Tensile strength of biochar/PET composites by the multiple interfaces between fiber and matrix. Hence the
was found to be much higher than neat PET, with the highest improvement in flexural strength was attributed to stronger
tensile strength being that of 0.5 weight% biochar/PET com- interfaces. Recycling processes delivered additional melting
posite (32 % higher) indicating the excellent bonding between impregnation functions so that the interface could be stronger.
PET and biochar. The values tend to decrease with additional The modulus however decreased a bit which was probably due
biochar content owing to the agglomeration of biochar particles. to the degradation of matrix during the recycling process. Flex-
The tensile modulus, however, was found to increase with ural strength and modulus of 3D printed composites were
more biochar content with 5 weight% having maximum value higher than that of solution preimpregnated and hot-pressed
(60 % higher). DSC analysis showed that the cold crystalliza- specimens with similar carbon fiber content of 25 vol%. How-
tion temperature decreased with biochar content hence proving ever, the flexural modulus was still lower than that of high car-
biochar as a nucleating agent while melting behavior remained bon fiber content. Unlike tensile strength shown in Fig. 18, the
unaffected. Biochar was also found to increase the crystallinity. impact strength of the originally printed CF/PLA (34.5 kJ/m2)
TGA analysis suggested good enhancement in the 5 and 30 % didn't exhibit a multifold improvement over pure PLA (20.0
weight loss temperatures with the addition of biochar, hence kJ/m2). The low failure strain of carbon fiber may cause the
suggesting better thermal stability due to barrier effect of bio- limited improvement in impact strength. No obvious improve-
char to volatiles. DMA analysis showed an increase in the stor- ment was obtained after recycling and remanufacturing. More-
age modulus with more biochar content with the highest one over, if compared with tensile and flexural strength, interlaminar
being for 5 wt% biochar. Calculation of tanδ (ratio of loss shear strength was quit low due to the character of layer-wised
modulus to storage modulus) suggested elastic behavior for fabrication for 3D printing.
composite and a viscous behavior for neat PET. The glass Pan et al. [53] studied the influence of nanocrystalline metal
transition temperature also increased with increase in biochar powders namely iron-silicon (Fe-Si), iron-silicon-chromium (Fe-
weight percentage. Further TMA analysis suggested an in- Si-Cr) and iron-silicon-aluminium (Fe-Si-Al) on the physical and
crease in the dimensional stability with biochar addition. mechanical properties of recycled polymers for FFF applica-
Tian et al. [52] researched recycled carbon fiber reinforced tions as shown in Fig. 23. HDPE/ PP polymers were obtained
polylactic acid composites for FDM printing. The recycling from containers, bottles, tubings and sent for recycling in fac-
process involved remelting the matrix of the 3D printed com- tory. The presence of nanocrystalline powders increased ther-
posite with the help of a hot air gun. This was followed by mal stability which was shown in the increase in the onset tem-
gradual and continuous pulling of the carbon fiber. The surface perature of degradation in TGA. This was explained by metal
of the filament was smoothened by a remolding nozzle. Finally, powders restricting the chain mobility of polymers hence a
the reimpregnated filament was fed to the 3D printer for re- higher energy for thermal decomposition is required. Addition
manufacturing. The continuous fiber reinforced composite of 1 % metal powders enhanced the young’s modulus and
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yield stress of the recycled materials. Also, Fe-Si and Fe-Si-Cr CLTE variation most for the 3D printed samples. The effect of
gave a stronger and more ductile material while Fe-Si-Al gave these printing parameters on the mechanical properties was
stronger but brittle material. In conclusion the recycled blends discussed. It was found that the mechanical properties for 3D
containing Fe-Si-Cr gave best results both according to physi- printed samples were comparable to injection molded samples
cal and mechanical characterizations. when the printing parameters are optimized.
Morales et al. [54] developed a sustainable composite fila- Tao et al. [29] utilized waste office paper (WOP) as fillers in
ment using rice husk (RH) as natural fiber in recycled polypro- the PLA matrix with a ratio of 5, 10 and 15 % WOP content.
pylene matrix (rPP) for FFF printing. A series of characteriza- The printed office paper was grinded using a ball mill machine
tions were performed to evaluate various properties of the 3D and sifted using a sieve. Silane coupling agents were used to
printed specimens. Recycled polypropylene pellets were ob- bind the filler with the matrix. The PLA-WOP filaments were
tained from post industrial waste and the size of the rice husk successfully 3D printed with FFF printer. The morphology of
was reduced using a Pulverisette 19 mill. the PLA-WOP composites showed lower filler dispersion and
Characterization of physical properties suggested a de- interfacial adhesion between the filler and matrix with the in-
crease in density with increasing fiber content due to the lower crease in WOP content due to the presence of larger voids,
density of the fiber. Further, the rPP/RH composites had higher fiber pull-out and debonding. The interfacial adhesion was
water absorption and swelling diameter than neat rPP because improved with treating WOP filler with a silane coupling agent
of the hydrophilic behavior of the RH. The TGA analysis (KH570). Due to the addition of KH570, less number of voids
showed that although the rPP/RH composites started degrad- were found and a smoother fracture surface was observed.
ing earlier than rPP because of lignocellulosic contents in the Rheological analysis showed a decrease in the complex vis-
fiber, they were capable of maintaining their thermal stability cosity of the composite with higher WOP content which meant
during the 3D printing process. The DSC analysis suggested improved melt flow. The storage modulus and loss modulus
that the composites had a lower crystallization rate than neat tend to decrease with higher WOP content while the compos-
rPP hence indicating reduced warping in the case of compos- ites containing KH570 showed higher complex viscosity, stor-
ites’ printing compared to neat rPP. The crystallinity however age and loss modulus indicating better interaction between
increased for 10 weight percent composite showing that the PLA and WOP. The DSC data showed a decrease in Tc value
fiber may act as nucleation sites at that weight percent. the with more WOP content showing more ordered structures with
mechanical properties were compared for two different raster addition of WOP. The increase in Xc (percent crystallinity) with
angles (0 and 90°). For 0° specimens, neat rPP had higher higher WOP content further showed an increase in crystallinity
stiffness, toughness and tensile strength than composites, this with WOP and the nucleation effect of WOP fillers. Silane treat-
was attributed to absence of chemical bonding and low disper- ment further enhanced the nucleation effect as well as crystal-
sion of fiber in the matrix which was also confirmed by the SEM linity of the blends. The decomposition temperatures from TGA
images. While for 90° specimens, there was more ductility and analysis showed a decrease with addition of WOP compared
higher energy absorption capacity in the material in the case of to pure PLA indicating lower thermal stability. Silane treatment
10 weight percent RH composites. improved the thermal stability, and the residues of PLA-WOP
Maldonado-García et al. [55] used recycled ocean plastics composites were higher than pure PLA due to the presence of
blend as matrix and biocarbon as filler for FFF 3D printing. The CaCO3 particles in WOP. The tensile strength of composites
plastic blend comprised of recycled HDPE and recycled PP. was decreased with addition of WOP filler because of the lower
They were bought from Oceanworks, USA. The MFI value for filler aggregation and poor interfacial adhesion between filler
the blend was found suitable for 3D printing, addition of 20 % and matrix. Silane treatment improved the tensile strength by
biocarbon reduced the MFI value by creating a reduction in the 9.5 % and elongation at break by decreasing the polarity of the
polymer chain mobility. The storage and loss moduli of the fibers.
blends and composites increased with higher angular fre- Gaikwad et al. [56] utilized e-waste plastics for the prepara-
quency. The composites containing 20 % biocarbon with and tion of filaments for FFF printing. The shredded e-waste plas-
without 2 % compatibilizer showed a reduction in the storage tics were obtained from printers. Polycarbonate was selected
and loss moduli as compared to rHDPE/rPP blend. Addition of as the subject for the investigation because it was found to be
20 % biocarbon showed reduction in percentage crystallinity the most dominant plastic in the e-waste sample. Further size
from DSC analysis. The 3D printed samples showed crystalli- reduction/granulation was done using a knife mill and drying in
zation and melting peaks at similar temperatures compared to an air-drying oven. The authors compared the properties of the
the injection-moulded ones, with the crystallization peak being filament and 3D printed parts with those of commercial ABS
somewhat broad which was attributed to the formation of im- virgin filament. The breaking strength of both virgin and recy-
perfect crystals owing to higher nozzle temperature. Addition of cled filament decreased as the number of processing cycles
biocarbon filler reduced the CLTE value of the composites due increased, with the reduction being higher in the case of e-
to the hinderance in polymer chain movement. The effect of waste plastic. As for the 3D printed samples, the e-waste 3D
bed temperature, nozzle temperature and line pattern was printed part was able to achieve 83 % of the tensile strength of
observed and it was found that the line pattern affected the the virgin plastic 3D printed part. The TGA analysis did not
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show much difference in degradation pattern for the virgin plas- observed in the case of e-waste plastic. This was expected as
tic after four processing cycles, while a decreasing trend was PC is more prone to oxidative degradation than ABS and the e-
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waste polymer had already undergone at least one thermal resulted in more consistent prints. However, too much increase
processing cycle. Also, a life cycle assessment of both plastics could lead to degradation. Other factors such as print orienta-
suggested that using e-waste PC resulted in 28 % reduction in tion and raster angle also affect the print quality. As an exam-
CO2 emissions compared to virgin ABS plastic. ple, the percentage decrease of ultimate tensile strength in Ref.
Table 4 presents a summary of the above studies. Common [22] was lowest for X build orientation.
recycling methods for plastics include mechanical recycling, The research studies contain information about different
chemical recycling and incineration. Chemical recycling in- types of recycled polymers, with or without fillers or other addi-
volves processes such as pyrolysis which breaks down the tives, and the resulting mechanical and thermal properties of
polymer into smaller units by heating it without oxygen. Incin- the printed parts. All of these polymers have their advantages
eration, refers to burning of these materials and using the re- and disadvantages in terms of how they are recycled, ease of
sultant heat for electrical and thermal energy. These processes, FDM/FFF printing, degradation of properties, print quality etc.
however, require high amount of energy, which is not entirely Based on these studies, it can be said that PLA and PET plas-
beneficial from both economic and environmental point of view. tics show good potential for efficient recyclable materials for
Mechanical recycling offers greater efficiency in terms of en- FDM/FFF printing. PLA is a biobased and biodegradable plas-
ergy and cost. Mechanical recycling of plastics includes proc- tic which makes it harmless for the environment. Its low melting
esses such as separation, washing, drying, grinding, shredding, point and easy processability makes it a suitable choice for
melting [6, 22, 23, 26-28, 75, 76]. Based upon the plastics and FDM printing [48]. The parts produced with recycled PLA show
the available technology, different recycling companies use good dimensional stability and surface finish. Although there
different techniques. As this review paper focuses on recycling exist several issues which can restrict its large-scale recycling,
materials for 3D printing, based on a review of the above stud- such as reduction in mechanical properties which can be a
ies, it can be seen that recycling of plastics such as ABS, PE, result of reduction in molecular weight during recycling [49].
PET, PP, PLA, nylon-6 comprises of some common steps However, addition of fillers such as carbon fiber or polydopa-
including sorting and cleaning of the material obtained from mine, along with optimization of printing parameters can im-
sources such as waste plastic bottles, milk cartons, waste 3D prove the mechanical properties so that it can be reused or
prints, waste support structures. The material is then reduced recycled to form value-added products.
in size using different techniques. Based on the material, they PET is an easily recyclable material [50] and despite of fac-
are either directly cut, chopped, grinded and crushed. They are ing some degradation during processing, its thermal properties
then shredded using electric shredder / paper shredder. The have found to be comparable to commercial PET. Its mechani-
plastic is then re-melted and re-extruded into filament for 3D cal properties can be improved by addition of fillers such as
printing [6]. There are several factors that influence the quality biochar. Studies have even shown improved crystallinity in
of the parts made by recycled filaments. The filament diameter recycled PET compared to virgin one [50]. Plastics such as
should be in the range applicable for 3D printing. The desired ABS, HDPE, PP also show potential for good recyclability,
diameter range for FDM printers is 1.7 - 1.8 mm which ensures however, improvement of mechanical properties of ABS
a continuous feed rate and hence consistent print quality [44]. through reinforcements needs to be explored. HDPE and PP
The dimensional stability of the strands also plays an important generally have difficulty in 3D printing due to warping and poor
role in ensuring good quality for the printed part. MFI is another adhesion to the print bed. Hence, they require adjustments in
factor that strictly needs to be kept in the desired range for printing processes such as heated print bed for consistent print.
proper printing in FDM. If MFI is too high, it can lead to over- Blends of ABS with other polymers such as HDPE have been
extrusion of the material on print bed. Addition of fillers has studied, however proper mechanical and thermal characteriza-
been found to reduce the MFI value by restricting polymer tion needs to be explored.
chain mobility. However, too low value can cause non-
uniformity in the flow and clogging of the nozzle [55]. An opti-
4.2 Case studies for recyclable resins for SLA/
mum fiber or filler content ensures proper flow velocity of the
DLP printers
filament resulting in good print quality and dimensional stability
in the samples [51, 55]. SLA/DLP printers offer advantages over FDM technology;
The printing parameters such as extrusion temperature, ex- they produce parts with smoother surfaces and higher resolu-
trusion width, screw speed, nozzle diameter have an impact on tions, as well as faster manufacturing. However, the resins
the parts produced with recycled materials. The temperature of used in these printers tend to be expensive [41].
the extruder from which filaments are produced influences the Some relevant research work focus on converting waste
filament diameter/thickness. Increasing the temperature leads cooking oil into 3D printable resins for SLA/DLP printers [41].
to higher melt flow while too high temperature can lead to Direct disposal of cooking oil is not good for the environment,
thermal degradation. Hence monitoring the extrusion tempera- as it contains unsaturated fats, and if disposed in the sewage it
ture is necessary to keep the diameter in the desired range of can lead to clogs from fat buildup. As shown in Fig. 19, waste
3D printing applicability [22, 44]. For example, in Ref. [44] in- cooking oil was collected from McDonald’s restaurant, and a
creasing the extrusion temperature from 230 °C to 235-240 °C one-step acrylation reaction was used to convert it into a 3D
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
equilibrium is achieved. Dynamic mechanical analysis was breaks down the polymer network into chain segments (180 °C
carried out to test its reshapability. It showed that there was a for almost 6 hours), the fully dissolved polymer solution was
steady increase in rubbery modulus from 0 to 4 hours after shifted to a vacuum oven at 180 °C followed by evaporation of
which it didn’t show a further increase. Suggesting that DCBs excessive solvent which left partially cured ink with appropriate
reached a state of dynamic equilibrium after 4 hours. The glass viscosity. The printed structures held their shapes after curing
transition temperature (Tg) also increased as DCBs increased, and even though slight shrinkage was observed, the printed
as the chain mobility gets restricted on incorporation of more structures were able to maintain their microprofiles after curing.
cross-links. This increase in Tg results in the material becoming In the second layer, single-layered walls of epoxy maintained
stiffer at room temperature, as the glassy state is stretched to a the shape during curing. While the third cycle showed some
higher temperature region. The authors also tested the repair- rough and grooved surface which was fixed by using nanoclay-
ability by replacing one of the lost ears of a 3D printed rabbit. A free epoxy vitrimer glue, the fourth cycle further showed good
flat surface was first achieved by polishing the damaged site. resolution printing hence showing great recyclability of vitrimer
3D printing was then done on the polished surface to replace epoxy. DMA results show that the glass transition temperature
the missing part. In order to gain the original mechanical per- of 18 weight percent nanoclay reinforced epoxy was close to
formance, thermal treatment was done (180 °C for 4 hours). that of neat vitrimer epoxy whereas much higher storage
Also, a strip was printed with a circular hole for a mechanical modulus (both rubbery and glassy) was observed showing the
flaw simulation. The hole was filled with reprocessable thermo- good reinforcement of nanoclay. Stress relaxation tests were
set solution, then UV light irradiation followed by heating. It was also conducted which showed that the epoxy network was able
found that repaired sample recovered almost 100 % stiffness to release the internal stresses by increasing the temperature.
and most of the strength (93 %). However, the mechanical The relaxation curves for third cycle were similar to first cycle
performance of 3DPRTs was less compared to traditional hence showing the recycled material’s network adaptability.
thermoset 3D printing materials and the authors suggest incor- Further, FTIR results proved the existence of dynamic equilib-
poration of non-covalent sacrificial bonds, nanoparticles and rium. Tensile tests reveal an increase in elastic modulus and
fibers to improve their mechanical performance. The authors ultimate strength for nanoclay reinforced vitrimers compared to
also checked the recyclability of the samples, which was done neat ones while ultimate stretch showed some decrease. Re-
by first grinding the printed structure into powders, pouring it cycled materials showed similar mechanical properties with
into a mold followed by thermal treatment. It was found that the only slight degradation.
recycling process was repeatable and the overall mechanical Zhu et al. [62] reported recyclable and self-healing polymer
performance of recycled samples was rather good in spite of resins, with urethane monoacrylate (UMA) and acrylic acid
small degradation. (AA) as monomers along with cross-linker and photoinitiators,
Shi et al. [61] performed another research that utilizes the which can be DLP printed. There was ionic bonding as well as
concept of vitrimers. Vitrimers are materials that contain the hydrogen bonding which could be broken reversibly through
properties of both thermoplastics and thermosets, that is, they varying temperature. This dynamic nature of the bonding ren-
are solid cross-linked structures at room temperature, like dered the self-healing and recycling ability to the resin. The 3D
thermosets, while at elevated temperatures, bond exchange printed dog bone samples were cut into two pieces and joined
reactions (BERs) take place which are reversible in nature, and together for varying periods at varying temperatures. The au-
hence dynamic covalent bonds (DCBs) are formed making the thors varied the ratio of the monomer (UMA/AA) to achieve
polymer network reversible or reprocessable and malleable, tailorable mechanical properties from soft elastomers to rigid
like thermoplastics [22, 24]. In this study, an epoxy vitrimer ink plastics. The UMA/AA ratios from 10:0 until 5:5 showed good
was developed to attain fully recyclable thermosetting polymer polymerization rates and low viscosities for DLP printing. There
3D printing. The 3D printing technique used here was direct- was a reduction in polymerization rates with additional AA. It
ink-writing (DIW) in which the resin is extruded through a noz- was observed in the DMA analysis that the storage modulus
zle which is attached to a syringe. The ink needs to have high and glass transition temperature (Tg) both increased with AA
viscosity so that it can hold its shape when it leaves the nozzle content. Increase in Tg was attributed to increase in the hydro-
and especially when the temperature is raised to curing tem- gen bonding. The stress-strain diagrams confirmed the highly
perature. The viscosity was increased by adding nanoclays tailored mechanical properties with different monomer ratios.
along with pre-crosslinking the epoxy (at 130 °C for 30 min in a The Young’s modulus and tensile strength showed significant
vacuum). This viscosity was good for curing temperature increase (from 0.1 to 172 MPA and 0.2 to 21 MPA, respec-
(130 °C) but not for room temperature, hence two flexible heat- tively) whereas the elongation at break showed reduction (from
ing elements were wrapped around the syringe and nozzle to 423 % to 12 %) with increasing AA content. The shore hard-
increase the temperature and hence reduce ink viscosity for ness also increased considerably hence giving varying resins
easy extrusion. Lastly, a two-step curing method was utilized. from soft elastomers to rigid plastics. The 3D printed speci-
The recyclable ink for second and more printing cycles, was mens were cut and then brought together at 90 °C for 12 hours
made by dissolving the entirely cured printed samples from the for self-healing. The 3D-printed model could be well-recovered.
preceding cycle. Ethylene glycol was used as solvent which The healed soft sample (UMA/AA ratio at 9:1) showed good
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
for 5 min under a pressure of 2 MPa. Chemical recycling in- original FPU samples. This recovery increased to more than
volved solubilizing the photopolymerized thermosets in ethyl- 80 % at a moderate temperature of 60 °C. The recycled FPU
enediamine followed by precipitation in water, vacuum filtration, was able to show similar tensile properties as the original one
vacuum oven drying, magnetic stirring in round bottom flask for at least three cycles. They also added fillers to the FPU and
along with few other materials and hot pressing in a square found that the composite maintained its conductivity and me-
mold. Both the resins X-SB1 and X-SB2 were found to be chanical properties during recycling. Further, they prepared
thermally stable in TGA. Both had higher values of glass transi- three FPU based devices via 3D printing to demonstrate its
tion temperatures than vanillin thermosets according to DSC. A recyclability and found that the recycled materials showed very
successful welding of X-SB2 was achieved owing to the imine similar mechanical properties as the original ones.
linkages. The self-healed sample showed a little increase in the An outline of above-mentioned researches is provided in
modulus while mechanical and chemical recycling did not show Table 5. The SLA/DLP printers require quick transitioning from
much difference in the elastic modulus. This increase in liquid to solid under irradiation. Hence monomers with multiple
young’s modulus was explained through the FTIR spectra, due functional groups are required. This is why these printers use
to additional thermal curing in the case of self-healed X-SB2. thermoset resins that are cross-linked and contain covalent
On the other hand, all the reprocessed samples showed some bonds. However, their highly dense cross-linked structure
reduction in strain and stress at break, in the case of self- makes them very difficult to recycle as they cannot be
healed and mechanical recycled samples, this was also ex- remelted by heat or solvent. Examples of thermosets include
plained by the FTIR spectra due to imine bond opening along epoxies, polyesters, polyurethanes, phenolics. Their common
with only partial compensation of curing completion, hence recycling methods include incineration, chemical, thermal and
decreasing the rigidity of the network. Their thermal characteri- mechanical recycling. Like thermoplastics, recycling thermo-
zation (TGA) showed good thermal stability upto 250 °C and a sets using incineration for energy recovery is not efficient as
higher than 24 % residue (w/w) at 600 °C. DMA results did not harmful gases are released into the environment. Their me-
show any great differences in the Tg values for reprocessed chanical recycling includes reducing the size of the waste
samples with self-healed and chemically recycled ones show- thermoset materials and grinding them using milling machine
ing somewhat higher values. Narrower curves or more defined such as ball mill. However, the fillers and matrix so obtained
glass transition temperature values indicated presence of uni- cannot be used to reprocess the thermoset material due to its
form network compared to original sample. Successful DLP low mechanical performance. Chemical recycling involves
printing was achieved for the SB2 resin with a good printing degradation of the 3D cross-links by means of solvents. How-
accuracy. ever, this can also require catalysts and is not considered very
Chen et al. [60] used an acrylate-epoxy hybrid resin intro- sustainable from economic point of view due to the involve-
duced with dynamic bond exchange reactions (BERs) in order ment of hazardous solvents [78]. The recent studies, as men-
to produce recyclable thermosets for DLP printing. They were tioned, utilize dynamic exchange bonds (DCBs) which are
able to print high quality and complicated designs. After ther- reversible covalent bonds such as Dials-Alder bonds, Schiff-
mal treatment, the PT73 (PT ratio 7:3) was able to support base linkages, ester bonds, ionic and hydrogen bonds. These
much higher weight than without thermal treatment. The types of reversible cross-links render reprocessability and self-
young’s modulus and tensile strength also increased signifi- healability to the thermosets. This yields products that are
cantly after thermal treatment because of the epoxy network good in quality and comparable in other properties to com-
curing. The printed polymers showed much higher tensile mercial resins, hence providing a new way for waste reduction
strength and young’s modulus, after the second epoxy network [2, 57, 79].
was introduced, as compared to the pure polymer resin. The In the studies mentioned for DLP printing, researchers have
glass transition temperature from DMA analysis for printed incorporated bond exchange reactions in different resins in
polymers ranged between pure acrylate and epoxy resins. order to reprocess thermosets. Thermoset resins such as vanil-
In another interesting study conducted by Guo et al. [13], the lin-based epoxy, epoxy vitrimer, polyurethane acrylates, com-
authors prepared a fully recyclable polyurethane elastomer bination of urethane monoacrylate with acrylic acid and
(FPU-furan containing polyurethane) containing dynamic cova- photoinitiators, show successful recyclability and good quality
lent bonds through Diels-Alder adducts. The DA adduct had printed parts. Incorporation of DCBs not only rendered self-
the ability to dissociate upon heating and reassociate during a healability and recyclability to these resins, it also increased
sufficient time frame at ambient conditions. Hence it became glass transition temperature, hence making them stiffer. Multi-
the first reported thermoset elastomer which could be fully re- ple recycling was achieved in all these resins without significant
cycled at room temperature without any chemical treatments to degradation in mechanical properties. Addition of fibers and
decompose the polymer chains. They prepared three types of nanoparticles was found to further improve their mechanical
FPU based flexible electronics - a position sensor, motion sen- and thermal properties. Utilization of waste cooking oil for 3D
sor and a flexible keyboard in order to demonstrate the recy- printed resins is also an innovative way for its recycle and fur-
clability of the design. The self-healed samples showed 50 % ther research on improving the mechanical properties of the
recovery of tensile properties at room temperature compared to resulting resins made with waste cooking oil can be explored.
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
Printer Recycled material used Print quality Characterization and testing Sources
Reduction in glass transition
Solus DLP 3D Good resolution, comparable to
McDonald’s waste cooking oil temperature, increase in storage modulus, [41]
printer commercial resins
good biodegradability
Tensile strength, toughness
DLP FreeEntity Excellent dimensional accuracy,
Dental powder comparable to PMMA compressive proper- [77]
Tech Inc. low surface roughness
ties better than PMMA
Increase in rubbery modulus and glass
Commercial DLP
Thermoset polymers Complex architectures printable transition temperature from 0 to 4 hours, [30]
3D printer
somewhat less mechanical performance
First, second cycles – maintenance of
In house shapes and microprofiles Increase in elastic modulus and ultimate
Nanoclay reinforced epoxy vitrimer ink [61]
built DIW 3D printer Third cycle – rough surface strength, decrease in ultimate stretch.
Fourth cycle – good resolution
Urethane monoacrylate (UMA) and Increase in Young’s modulus, tensile
Homemade desktop Good polymerization rates,
acrylic acid (AA) along with strength, shore hardness [62]
DLP 3D printer low viscosity
cross-linker and photoinitiators Decrease in elongation at break
Photon Ultra DLP Polyurethane containing Successful depolymerization of printed
Identical to original resin [63]
printer hindered urea bonds materials without any catalysts or solvents
Commercial DLP Consistent storage modulus, tanδ
Isobornyl acrylate (IBOA) Good polymerization rates [57]
printer Good recycling efficiencies
UnionTech, S110 Polyurethane acrylate based on Similar tensile strength, reduction
Excellent resolution and accuracy [58]
DLP printer diels-alder bond in elongation at break
Commercial DLP
Vanillin based resin with imine bonds Good accuracy Similar modulus, good thermal stability [59]
printer from ASIGA
Homemade DLP
Acrylate epoxy hybrid resin High print quality Higher tensile strength, young’s modulus [60]
printer
BS4.2 DIW printer Furan-containing polyurethane (FPU) Stretchable, complex curves printable Higher tensile strength recovery at 60 °C [13]
For vat photopolymerization techniques, the time of expo- which hence filled the area between the two peaks of the bi-
sure to the light source plays an important role, as the layers modal distribution, hence resulting in a monomodal one for
need to adhere properly to the platform as well as to other reused powder. They also tested the chemical composition of
layers. The temperature needs to be increased for a time dura- the various powders which showed very similar values com-
tion so that dynamic exchange reactions can occur for recy- pared to the values in data sheet, indicating identical composi-
cling of thermosets [60]. The layer thickness also tends to af- tions for the powder particles and hence a homogeneous ma-
fect the mechanical and morphological properties of printed terial. Further, the virgin and reused powder showed very simi-
parts. lar values. They also calculated the PREN number (pitting
resistance equivalent number) that indicates how resistant a
material is to seawater. The virgin powder showed a value of
4.3 Case studies for metal 3D printing
37.3 which increased to 38.1 after reusing both of which are
Hilzenthaler et al. [31] examined how the properties of a su- much higher than 32. Further, the reused powder showed in-
per austenitic steel AISI 904L change due to reusing of powder. crease in flowability indicating a smoother surface which could
They reused the powder upto 10 times by sieving the excess be seen from the lower avalanche angle in the case of reused
powder with a mesh size of 50 μm and using it again in the powder. As a result of that, the dynamic density also increased
next cycle. They conducted various tests such as particle size (Fig. 23). The dynamic density of oversized particles was low-
distribution, melt flow behavior and electric properties. They est, however, due to larger gaps between particles and lesser
also analyzed the oversized particles as they can give informa- number of fine particles. There was a marked difference in the
tion about the influence of laser energy on the particles. The electrical impedence spectroscopy between the virgin and
particle size distribution curves showed no significant differ- reused powder due to the presence of oxides on the surface of
ence between the virgin and the reused powder. powder. Further, mechanical tests of specimens made from
Only a slight variation was observed in the fact that virgin both virgin and reused powders were conducted and the val-
powder showed bimodal particle size distribution while reused ues were compared with data sheet values. The values for
powder showed a monomodal one. This was explained by the tensile tests were higher than those from data sheet while the
occurrence of some spatter in the 20 to 40 μm size range yield strength, elongation at break and ultimate tensile strength
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
Fig. 24. PSD for fresh and recycled AlSi10Mg powders [34].
Fig. 23. Results from revolution powder analyzer [31].
The fabricated parts were then tested for porosity which re-
were close to the values from data sheet with only little stan- vealed similar porosity for different iterations (close to 0.10 %)
dard deviation. Hence multiple recycling does not cause any hence indicating that the fabricated parts had homogeneous
difference in the mechanical properties. properties. The mechanical properties were estimated through
Yi et al. [32] examined the effect of In718 powder reuse on Charpy impact tests and no apparent correlation was observed
the final SLM manufactured parts. They analyzed the pore between different iteration values.
evolution mechanisms, microstructures and the mechanical Maamoun et al. [34] used reused AlSi10Mg powder for the
properties of the parts. The particle size distribution (PSD) fabrication of SLM produced parts and the microstructure
studies after 2nd, 6th, 10th and 14th reuse times showed a shift of analysis, effects of thermal post-processing as well as micro-
the peak to the right indicating an increase in the average par- hardness was evaluated. They studied the reuse of powders
ticle size of the reused powder. Their morphology showed an for 18 build cycles and sieved the powder using a 70 µm mesh.
increase in the particle size after the 14th reuse time, which was Characterization of powder showed that the PSD curves of the
consistent with the PSD results. The chemical composition of fresh and reused powders were very similar (Fig. 24). The
the reused powder was same as the virgin powder. There was SEM observations showed spherical particles for fresh powder
an increase in the apparent density of the reused powder sug- while slightly elongated particles for the reused powder. The
gesting efficient packing in the reused powder. The flowability spherical shape leads to better flowability and higher apparent
also increased with the increase in reuse times. This was at- density. The chemical composition of both powders was almost
tributed to the decrease of small-size powder which would not same through EDS analysis. The reused powder surface did
allow agglomerate formation because of high friction between not show much evidence of more oxide formation, hence pow-
particles. The effect of reuse times on the pore defects was der characterization showed similar properties for both fresh
analyzed using the CT technique on the final In718 parts pre- and reused powders. The microstructure of the fabricated parts
pared using reused powder. With the increase of reuse times, using both powders was similar to that reported in literature.
an overall increasing trend was observed, specifically for de- The micro-hardness did not show any significant difference in
fects with deq less than or equal to 50 μm. The sphericity of the the build direction for the reused powder part, however it in-
defect also improved with reuse time. Also, the porosity (vol- creased with an increase in the building height. The effect of
ume of defects) showed an increase with the reuse time. The thermal post-processing on the fabricated parts using reused
reuse times did not have any significant impact on the me- powder would be useful for industrial applications that require
chanical properties as it was found that the ultimate tensile high ductility and low hardness.
strength, elongation at break and yield strength remained al- Zapico et al. [35] reused 17-4PH stainless steel powder for
most same from 0 to 14th reuse time. SLM manufacturing. The reusing process was done by apply-
Ardila et al. [33] reused In718 powder for SLM part fabrica- ing vacuum and sieving the powder. The chemical, morpho-
tion and analyzed its behavior through several iterative proc- logical and microstructural properties at different stages of
esses. The iterative process is described as fabrication of test reusing (10 and 20 reusing cycles) were compared with the
sample from the virgin powder in the first step, followed by original powder. The average diameter of the 20 times reused
sieving and drying the residual powder, a part of which was powder was higher than the virgin powder in PSD analysis.
studied for its properties and the rest was sent again to repeat There was also some decrease in the average roundness and
the fabrication process. The SEM images and particle size average aspect ratio after 20 uses which was much less sig-
distribution suggest that particles tend to aggregate with in- nificant after 10 uses. This can affect the fluidity of the particles
creased number of iterations. The chemical composition was in the SLM process. The amount of irregular shaped particles,
studied through energy-dispersive X-ray spectroscopy which agglomeration of particles increased with increasing number of
showed no difference between the first and the last iterations. uses. In the case of chemical composition, IGFT analysis did
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
not show much difference in the oxygen concentration (be- printed cubes also did not show any significant variation among
cause of thermodynamically stable oxides). The EDS analysis different reuse cycles. Ti-6Al-4V showed some increase in
however showed higher oxide concentrations in 15 µm larger oxygen level which explained the slightly higher strength and
particles. The XRD analysis showed some increase in the aus- reduces ductility in the titanium parts. Also, the drop in ductility
tenite phase for reused powder. for 17-4PH SS was explained by a possible increase in the
Giganto et al. [36] characterized the parts manufactured carbon content. Further, the fatigue properties were not af-
through SLM using the 17-4PH stainless steel powder of the fected by reuse of powder as the porosity remained largely
previous study. They compared the properties of virgin powder constant with powder reuse (as density of the part remained
with 20 times reused powder. There was a decrease in the constant).
porosity of parts made with 20 times reused powder by 0.16 % Asgari et al. [39] investigated the properties of recycled
compared to virgin powder. Also, the parts made with reused AlSi10Mg powder and compared them with virgin and conden-
powder were generally smaller in size and more circular. The sate powders for DMLS applications. The virgin powder was
powder reuse led to a decrease in roughness. The average received from EOS company. The samples were manufactured
hardness value for virgin powder samples was somewhat through DMLS process using the virgin powder and the reused
higher than the reused ones. While the ultimate tensile strength powder was obtained by sieving the unused powder using a 60
(YTS) in recycled powder samples was 54 MPa higher than µm mesh size. The powder that remained on the sieve due to
virgin, the YTS was lower for the reused powder parts. These its coarse size was used as the condensate powder. The pow-
results indicate an increase in ductility and hence a decrease in ders were studied for their morphology, particle size and
the hardness values. chemical composition. The SEM analysis indicated similar
Another study conducted by Popov Jr. et al. [37] researched morphology, spherical in nature, for recycled and virgin pow-
how reused Ti-6Al-4V alloy powder affects EBM manufactured ders. This led to good powder flowability, uniform packing den-
part quality. Half of the printed samples were subjected to HIP sity and layer thickness of the powder. The average particle
post-printing treatment (Hot Isotactic Pressure) which aims to size and microstructure of recycled powder was very similar to
eliminate the possible residual closed porosity. In the morphol- virgin powder. A comparison of mechanical properties revealed
ogy analysis of the reused powder, several defects were ob- comparable values for parts made from recycled powder com-
served such as agglomerates, elongated particles, broken and pared to those made from virgin powder, hence suggesting
non-spherical particles among others which could result in positive use of recycled powder in the DMLS process.
decreased flowability. The cause of the defects was mainly Sun et al. [40] conducted a study on reused Ti-6Al-4V pow-
attributed to the sieving procedure used, overheating and der for EBM 3D printing. There is a general trend of increase in
smelting of the particles. As for the microstructure of the EBM oxygen content in the case of Ti-6Al-4V with the number of
printed parts, not much variation was observed in the parts built reuses, hence the study emphasizes on how reusing affects
from recycled or virgin powder, both in as-built parts and HIP the accumulation of oxygen in the powder. The powder was
treated parts. The mechanical testing showed the elongation retrieved from the Arcam powder recovery system and it was
and reduction in area were very less for the reused powder sieved to remove the particles less than 40 µm and refilled into
samples compared to those made from fresh powder. Fatigue the Arcam machine. The morphology analysis of the virgin and
tests also revealed longer lifetimes in the case of parts manu- reused powders through SE SEM suggested elimination of the
factured from new powder. Both of these results were attrib- smaller particles (less than 10 µm) in the reused powder com-
uted to the residual surface oxidation and surface defects in the pared to virgin powder. The surface of the reused powder was
reused powder. It was found that HIP improved the fatigue found to be rougher and somewhat irregular compared to the
strength of the parts made from reused powder. smooth and spherical virgin particles. The PSD suggested a
Alamos et al. [38] utilized eight times reused 316L SS, 17- narrower size distribution for reused powder compared to the
4PH SS and Ti-6Al-4V powders in DMLS applications and virgin powder which was explained by the elimination of
evaluated the effects of print parameters on mechanical prop- smaller particles during reusing. Further, the mean oxygen
erties of printed parts. After each printing cycle, the unfused value in the case of reused powder (2050 ppm) was higher
powder was screened by means of a mesh sieve. A PSD than the virgin powder (1500 ppm). However, this increase in
analysis of the virgin and reused powders showed no signifi- oxygen did not lead to significant change in the surface oxide
cant differences in the case of 316L SS and 17-4PH SS while thickness in the reused powder compared to virgin powder.
the PDS for Ti-6AL-4V became narrower which was explained This was explained by the study of microstructures of the pow-
by the elimination of largest particles during sieving and re- ders. The metastable martensitic α′ phase of the virgin powder
moval of smallest particles because of dust collection. Me- got shifted to equilibrium α + β phase in the recycled powder
chanical testing of the printed parts showed some enhance- and the excess oxygen got primarily stored in the β phase.
ment in strength and reduction in strain to failure for Ti-6Al-4V Shanbhag et al. [64] conducted a study for the reuse of
while not much difference was observed in 316L SS and 17- plasma atomized Ti-6Al-4V powder in EBM 3D printing. They
4PH SS. The densities of the printed parts were not found to studied four types of powders, including virgin powder (G0), the
be dependent on powder reuse and the chemistry of the powder that was leftover after printing was sieved and used
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
again for the same 3D printer (G1). This process was repeated powders are generally reused in the same printing cycles.
again (G2) and finally a blend of G1 and G2 powders in equal Since only some amount of the powder melts and fuses to print
weight% was prepared (GB12). Their morphological analysis a part, reusing the remaining unused powder can solve two
using SEM indicated that powder reuse induced defects in the purposes, a) it helps in reducing waste, and b) it leads to sig-
powder in the form of broken and shattered particles, molten nificant amount of cost saving as metal powders are generally
satellites, deformed and elongated particles. The PSD of G2 expensive. The common strategy to reuse them includes siev-
powder was slightly broader than G0 powder while G1 and GB12 ing of the unused powder which was left after the printing proc-
showed narrower distribution. The flowability of all the reused ess, until its properties reach out of the pre-defined limits. The
powders and blend was found to be lower than the virgin one size of the sieving mesh is selected based on average PSD
because of higher particle interlocking resulting from angular analysis [80].
powders or less spherical powders. The oxygen content in However, the key concern lies in maintaining the properties
reused powders was higher compared to virgin one, because of the powders, such as flowability, apparent density, morphol-
of exposure to ambient conditions. This can lead to lower duc- ogy, average PSD, presence of satellites, presence of angular
tility and flowability of the powder. It was also mentioned that and elongated particles. These changes can in turn affect the
blend can have lower flowability than separate powder compo- quality of the printed part. If the flowability of the powder is not
nents. in the required range, it can lead to inhomogeneous layer den-
Cao et al. [65] focused on the morphology and surface sity, hence resulting in non-uniform layers which can even
chemistry of plasma atomized Ti-6Al-4V powder. They reused cause failure during the printing [64, 80, 81]. The packing den-
the powder for EBM process and analyzed the properties after sity of powder can affect the density of printed part by increas-
5 and 10 reuse cycles. Their morphology analysis through ing porosity. The PSD can affect layer densities as broader
SEM showed similar features in recycled powders compared to PSD can lead to higher density in the parts [64]. Agglomeration
virgin one, although some roughening of the surface was ob- and presence of satellites leads to changes in morphology of
served. According to XPS analysis (X-ray photoelectron spec- the powder, which can in turn impact the flowability. Hence all
troscopy), an increase in the oxide thickness was found due to the properties need to be maintained in order to print the part
recycling, along with some inhomogeneity. There was also a with desired quality.
reduction in Al concentration due to its high vapor pressure In the case of metal 3D printing, factors such as exposure
which led to its evaporation. Also, the higher affinity of Al to- time to the energy source, area of exposure, power of the en-
wards O, led to local oxidation and Al rich oxide formation at ergy source, exposure to humidity, contamination due to pres-
the surface. ence of debris in the chamber, sieving procedures, can all have
Table 6 presents a summary of the above studies. Metal an impact on the quality and mechanical, thermal and morpho-
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Journal of Mechanical Science and Technology 37 (11) 2023 DOI 10.1007/s12206-023-1001-9
logical properties of the printed parts. The height and volume of issue by adding reinforcements such as fibers, fillers and other
the build material needs to be maintained at a desired level, as waste materials. However more research in this area is re-
due to powder reuse, there can be decrease in the printable quired. Issues such as contamination due to impurities during
height after each build cycle [80, 82]. the recycling process can result in poor mechanical perform-
Reuse of stainless-steel alloys such as AISI 904L and 17- ance. The warping and poor adhesion of polypropylene and
4PH SS, aluminium and nickel alloys (AlSi10Mg and In718) in polyethylene can cause printing problems. The reduction of
SLM and DMLS 3D printing show positive results. All of them mechanical properties of ABS, which is one of the most com-
retain their chemical composition after reuse and the PSD in all monly used material in FDM, restricts its recycling. The printing
these reused powders is similar to the virgin powder. With the process needs to be optimized in order to produce parts with
exception of a little decrease in the flowability of AlSi10Mg due desirable quality and properties. For DLP printers, although
to presence of elongated particles, all the other powders mechanical and thermal properties from bond exchange reac-
showed increase in flowability which is good for metal 3D print- tions for resins have been found to show positive results, recy-
ing. As for mechanical properties, both AISI 904L and In718 cling techniques that can be applied on a large scale need to
showed similar mechanical properties compared to parts made be researched. The increase in oxide layer thickness in EBM
with virgin powder. However, the number of cycles until which printers remains a big challenge in reusing powders for EBM
they can be reused without out-of-limits degradation of proper- printers, which is because of exposure to ambient conditions
ties, should be carefully considered before using them for ap- during reuse.
plications. Reuse of titanium alloys such as Ti-6Al-4V has been
investigated extensively for metal 3D printing, in particular, for
EBM processes, however the reused powders generally have
7. Future perspectives
higher oxide formation, lower flowability and narrower PSD There is a lot of scope for future research in this area. A
values than virgin powders [80]. number of researches have been done using waste materials
such as waste office paper, waste tires, recycled sand, ocean
plastics, electronic waste, and preparing their composites with
5. Conclusions
polymers in order to yield filaments for FDM printing or resins
This paper presents a comprehensive review of the latest ad- using waste cooking oil for DLP printing. More such studies
vancements in the recycling of waste materials for 3D printing can be explored their mechanical, thermal, morphological
applications. It begins with a concise introduction to various 3D properties can be characterized and improved by various
printing techniques, including FDM, FFF, SLA, DLP, SLM, EBM, treatments such as silane treatments or coupling agents in
DMLS, and SLS. Additionally, it explores the commonly used order to reduce waste from the environment and produce
recycled materials in these applications. FDM and FFF 3D print- value-added products. Blends of ABS with various other poly-
ing processes predominantly employ thermoplastic filaments mers can be explored further so that the printed parts have
such as PLA, ABS, PP, and PE. When utilizing recycled fila- improved mechanical properties. More number of researches
ments, comparable surface finish and printing quality can be need to be conducted for recycling of plastics such as nylon-6,
achieved in contrast to virgin materials. Although the mechani- PA-12, PC by adding fillers and adjusting print parameters. The
cal properties may degrade, they can be enhanced through use of DCBs in thermosets seems like a very promising area
reinforcements like fillers and natural fibers, as well as surface for recycling of thermosets and needs to be explored more.
treatments. On the other hand, SLA and DLP applications typi- More studies need to be conducted in the area of SLA, SLS,
cally rely on thermoset resins like polyurethane, which pose DMLS and EBM printing incorporating different alloys. The
challenges in recycling due to their highly dense cross-linked increase in oxide layer thickness of titanium needs to be ad-
structures. To overcome this, the utilization of dynamic ex- dressed. By addressing these challenges and expanding re-
change bonds has emerged as a solution, providing materials search efforts, we can unlock the full potential of recycling in
with reversibility and self-healing properties. In processes such 3D printing, paving the way for a more sustainable and envi-
as SLM, EBM, and SLS, metal powders are utilized. Reused ronmentally friendly approach to manufacturing.
metal powders generally exhibit similar chemical compositions
and particle size distributions to virgin materials, resulting in
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