1. Introduction
In recent years, the global production of plastics has experienced a significant surge. As per the data provided by the Statista Research Department [
1], the yearly global production of plastics surpassed 390.7 million metric tons in 2021, marking an annual growth rate of 4% and indicating a continuing upward trend. However, the escalating production of plastics has been accompanied by environmental issues, such as the build-up of plastic waste in land and ocean ecosystems. An estimated range of 4.8–12.7 million tons of plastic waste is discarded into the world’s oceans on an annual basis [
2], resulting in severe marine contamination and constituting a substantial hazard to marine organisms. Furthermore, it is emphasized that of the 6.3 billion metric tons of plastic waste generated, a shocking proportion of 79% has piled up in landfills or the natural environment [
3].
As the magnitude of plastic production persists on its upward trend, there is an increasing necessity to mitigate the intricate environmental repercussions. Landfilling, as a temporary measure for plastic waste, remains inadequate in addressing the escalating plastic production and minimal recycling rates [
4]. Hence, there is an urgent need for plastic recycling technologies. Beyond existing methods, emerging technologies such as additive manufacturing (AM) using recycled polymers could be an innovative approach to reduce plastic waste.
AM, often known as 3D printing, has emerged as a revolutionary technology for producing functional components across various fields [
5]. Its ability to create complex geometries with high precision has positioned it as a preferred method for modern manufacturing [
6]. One of the key advantages of AM is its potential as a clean processing technology, especially when integrating post-consumer recycled polymers into the production cycle [
7]. This approach not only leverages the principles of the circular economy but also offers a significant solution to the escalating issue of global plastic contamination.
Research by Beltrán et al. [
8] explored the recycling potential of polylactic acid (PLA) from 3D printing waste. By examining the properties of recycled PLA film, the findings suggest that adopting a distributed recycling approach, which focuses on a consistent and well-characterized PLA grade, could yield mechanically robust recycled materials that remain compostable at the end of their lifecycle [
8]. Additionally, the study by Mishra et al. [
9] involved repurposing acrylonitrile butadiene styrene (ABS) waste plastic from post-industrial sources by blending it with virgin ABS pellets. These mixtures were extruded into filaments and demonstrated successful application in 3D printing through the fused deposition modeling (FDM) technique [
9]. Additionally, the efforts of Herianto et al. demonstrated promising results in recycling polypropylene waste into 3D printing filament using material extrusion [
10]. Similarly, research by Arrigo et al. successfully created a 3D printing filament by recycling polypropylene from urban waste and reinforcing it with talc [
11]. Further, Daliri et al. explored the potential of recycling polypropylene from mushroom boxes into 3D printing filament by mixing it with glass fiber, showcasing the versatility and viability of polymer recycling in additive manufacturing [
12].
However, efforts to recycle polymers into 3D printing filaments have predominantly focused on common materials such as PLA [
13,
14,
15,
16,
17] and ABS [
18,
19,
20,
21,
22]. These materials are well-studied and widely used in the 3D printing industry. However, there is a notable gap in research concerning high-density polyethylene (HDPE), despite it being a major contributor to plastic waste [
23]. Addressing this gap is crucial, as HDPE constitutes a significant portion of discarded plastics, particularly in the form of disposable water bottle caps [
24].
HDPE is a type of polyolefin polymer with only 5 to 10 short-chain branches per 1000 carbon atoms [
25]. As a semicrystalline polymer, when cooling from a molten state, HDPE often exhibits significant shrinkage due to the long-range ordering of polymeric chains [
25]. This material also suffers from considerable warpage and poor adhesion to the print bed, which can lead to print failures [
25]. Hence, advancing the creation of polyolefin filaments is crucial to enhance their versatility in design and manufacturing. While HDPE is usually processed using various common melt-processing methods such as injection molding and extrusion, the feasibility of recycling HDPE for use in AM has been documented, for instance, by Daniele et al. [
26]. The study evaluated the printability and mechanical performance of recycled HDPE, highlighting both the challenges and opportunities associated with its use in AM.
However, the majority of the research indicates that recycled filaments often show reduced mechanical properties [
27,
28,
29,
30,
31,
32]. For instance, a study by Charles et al. found that the mechanical strength of recycled ABS polymer decreases with each recycling cycle [
33]. Tensile tests revealed a gradual decline in maximum tensile stress and elastic modulus with successive recycling. While the initial drop in tensile stress from the original filament to the first recycled one is minimal, more substantial reductions occur in the second and third cycles. Specifically, Young’s modulus drops by 25% in the second cycle and 16% in the third cycle compared to the virgin material [
33]. The reduction in mechanical properties can be attributed to the chain scission of polymeric chains, leading to progressive embrittlement of the recycled material [
15]. Additionally, factors such as a reduction in chain length, lower molecular weight, and increased crystallinity collectively promote crack propagation [
15].
Therefore, enhancing the mechanical behavior of recycled filament is a key focus in recent research. One promising approach is the addition of additives to the base material. For example, Kristiawan et al. studied the effect of incorporating glass powder into recycled polypropylene (rPP) from food packaging for FDM filaments [
34]. Their results indicated that adding glass powder enhanced thermal stability and increased the melting temperature of the rPP. Furthermore, specimens with 10% glass powder showed significant improvements, with a 38% increase in ultimate tensile strength and a 42% rise in Young’s modulus compared to pure PP specimens [
34].
The present research aims to explore the properties of 3D printing extrusion using rHDPE derived from disposable water bottle caps. To enhance the material properties, different percentages of glass powder were incorporated into the HDPE matrix. This study focuses on validating the filament as a viable feedstock for commercial 3D printing extrusion equipment. The quality of the 3D printed objects was assessed through detailed microstructure observations and by comparing the mechanical properties of the printed specimens with those of commercially available 3D printable materials. Additionally, in this study, the potential application of rHDPE in sound absorption was explored, comparing its performance with commercially available materials. This aspect of the study opens new avenues for the utilization of rHDPE, particularly in applications where sound absorption is critical.
Finally, this investigation will not only advance the understanding of rHDPE’s potential in AM but also contribute to sustainable practices by promoting the use of recycled materials. By extending the life cycle of HDPE through its application in 3D printing and exploring its sound absorption capabilities, this research underscores the pivotal role of innovative recycling strategies in mitigating plastic pollution.
2. Materials and Methods
2.1. Materials
The rHDPE material utilized in this study was sourced from used water bottle caps. To prepare the material, the bottle caps underwent a thorough washing process to remove dirt and surface impurities. Subsequently, they were dried using sunlight exposure. Once completely dry, the caps were shredded into flakes with an average particle size of 5 mm using a shredder machine operating at 200 rpm. The glass powder, sourced from crushed glass and sieved through a mesh size of 200, was used for reinforcement. The rHDPE flakes were physically mixed with glass powder (GP) in various weight ratios, specifically rHDPE/GP at 100/0, 90/10, and 80/20.
2.2. Filament Extrusion
The extrusion process was carried out using a single screw extruder by Felfil Evo. Prior to initiating extrusion, the extruder barrel was preheated to 180 °C for 15 min to eliminate any trapped moisture within the setup. During the actual extrusion, the temperature was adjusted to various levels, ranging from 180 °C to 220 °C. Inside the extruder barrel, the material underwent softening and liquefaction. The softened material was then forced out through a 1.75 mm-diameter nozzle, which was then cooled down by an air fan.
Table 1 shows the extrusion parameters used in this study.
The design of the experiment employed the Taguchi method with an L9 orthogonal array, and each configuration (
Table 2) was repeated three times. The observed output was the tensile strength of the filament. In this project, the L9 orthogonal array accommodated three factors with three levels of parameters (as detailed in
Table 1). This design allowed for independent factor evaluation while minimizing the number of trials required. Once data were collected from the arrays, Taguchi analysis was conducted to guide the selection of parameter values to optimize the filament’s performance.
2.3. Differential Scanning Calorimetry (DSC)
A DSC experiment was performed to determine the melting point and degree of crystallinity of the polymer. The melting point illustrates the temperature span during which the polymer shifts from being rigid and somewhat brittle, akin to glass, to becoming soft and rubbery, while the degree of crystallinity describes the proportion of a material that has a crystalline structure. The degree of crystallinity (
) can be measured by calculating the ratio of the crystalline part of the semicrystalline polymer, shown in Equation (1). The experiment utilized a Mettler Toledo DSC1 apparatus, operating from 0 to 250 °C with a heating rate of 10 °C/min under ambient air conditions.
where
represents the heat of fusion of the sample, which is calculated from the area under the endothermic peak in DSC analysis.
stands for the heat of fusion of a fully crystalline material—in this case PE, with a value of 293 J/g [
35]—and
is the weight ratio of glass powder in the mixture.
2.4. Fused Deposition Modeling (FDM)
To fabricate the 3D printed specimens, an FDM commercial 3D printer CUBICON SinglePlus with a 0.4 mm nozzle was used. The rHDPE filament was compared to the commercial ABS and PLA filaments. The commercial filaments used were ABS-A100 and PLA-i21, both from CUBICON. The 3D printing parameters for the PLA and ABS material were based on their optimal parameters as adapted from [
36,
37].
Table 3,
Table 4 and
Table 5 show the printing parameters for ABS, PLA, and rHDPE filament, respectively.
2.5. Tensile Test
The tensile tests were performed using a universal testing machine, Instron 8874. Tensile tests were conducted for both filaments and 3D printed specimens. The filament with a length of 110 mm was clamped between the 3D printed gripper, which was attached on both tips of the filament (
Figure 1). The gripper was used to distribute the clamping force on the filament. The tensile tests were conducted with a 20 kN load and 5 mm/min speed until necking and stretching of the filament. Meanwhile, the 3D printed specimen followed the ASTM D638 standard [
38]. The dog bone specimen was tested with a 20 kN load and 5 mm/min speed until the specimen failed.
2.6. Flexural Test
Flexural experiments were performed on 3D printed samples of 125 mm × 12.7 mm × 3.2 mm by following the ASTM D790 standard [
39]. The specimens were loaded in a three-point bending grip mounted on an Instron 8874 universal testing machine. The span between the two supports was L = 20 mm (
Figure 2). Tests were performed with a 20 kN load, and crosshead speed of 2 mm/min, and the test ended at a displacement of 4 mm.
2.7. Compression Test
The compression tests were performed on 3D printed cylinders using a Shimadzu SFL-25AG machine by following the ASTM D695 standard [
40]. The specimens were tested with 20 kN load at 2 mm/min speed until the specimens failed.
2.8. Printed Part Quality
The final quality assessment of 3D printed specimens was conducted through microscopic observations and surface roughness measurements. The examination of the surface morphology and structural details of the printed samples was performed using the Keyence VHX−6000 digital microscope equipped with a magnification of 20 to 200 times. Additionally, scanning electron microscopy (SEM) was employed to further inspect the surface topography of the specimens. Meanwhile, to quantify the surface smoothness, surface roughness measurements were carried out using a Mitutoyo SJ−210 stylus profiler on 6 different points across the printed specimens.
2.9. Sound Absorption Test
The sound absorption test was conducted using the BSWA SW4601 series impedance tube to determine the absorption coefficient, adhering to the ISO 10534–2 standards. The investigation was conducted in a high frequency range, spanning from 500 Hz to 6400 Hz.
The samples for the sound absorption test were cellular diamond structures designed using MSLattice software. The sample design (
Figure 3) was a cylindrical shape with a 12 mm height and 28.5 mm diameter to fit the dimensions of the experiment apparatus. The structure had a 6 mm unit cell, 30% relative density, and 20% mesh.
2.10. Environmental Implications
The software used to perform the life cycle analysis was OpenLCA 2.0.2. For this study, the database used was the ELCD (European Reference Life Cycle Database) version 3.2. ReCiPe 2016 Endpoint Hierarchist version was selected as the methodology for calculating environmental impacts. The ReCiPe method is widely utilized in various research domains, particularly for life cycle analyses related to AM from a hierarchical cultural perspective. There are three different scenarios to compare, each with its flow details as follows:
Scenario 1: Cradle to incineration (
Figure 4a). Scenario 1 begins with the production of bottle caps at the factory. The raw material used for producing bottle caps is high-density polyethylene granulate (HDPE), a production mix, at the plant. The material is injection-molded into bottle cap form. The used bottle caps are then disposed of in the incineration plant.
Scenario 2: Cradle to landfill (
Figure 4b). Scenario 2 also begins with the production of bottle caps at the factory with the similar raw material of HDPE granule, which is injection-molded into the bottle cap. In this scenario, the used bottle caps are disposed of in the landfill.
Scenario 3: Cradle to filament (
Figure 4c). Like the two previous scenarios, Scenario 3 also begins with the production of bottle caps. The difference is that the used bottle caps are not disposed of but recycled instead. The used bottle caps are collected and undergo pre-treatment processes such as washing and drying, then shredded into flakes. After that, the plastic flakes are extruded into filament by the extrusion machine.
In this study, the transporting, packaging, and use phases were not considered since the environmental impact comparison was mainly focused on the production and end-of-life phase.
4. Conclusions
In this study, an experiment to recycle HDPE from bottle caps into 3D printing filament was successfully conducted. By optimizing extrusion parameters: setting the temperature at 180 °C, speed at 7 rpm, and incorporating 10% glass powder into the HDPE matrix, a filament with notable tensile strength averaging 25.52 MPa was achieved. To put this into perspective, this tensile strength was slightly higher than that of the ABS filament, which averaged 25.41 MPa, and was only marginally lower than that of the PLA filament, which averaged 28.55 MPa. While the filament exhibited some diameter inconsistencies, it was still usable in 3D printers and capable of producing printed specimens.
Comprehensive mechanical testing provided valuable insights into the performance characteristics of the rHDPE + 10%GP printed specimens in comparison to those made from virgin commercial filaments like ABS and PLA. The results indicated that the rHDPE + 10%GP specimens exhibited lower ultimate tensile, flexural, and compression strengths. Specifically, the average ultimate tensile strength of the rHDPE + 10%GP specimens was 13.94 MPa, which was notably lower than that of ABS at 26.93 MPa and PLA at 28.57 MPa. Similarly, in terms of flexural strength, the rHDPE + 10%GP specimens recorded an average of 41.15 MPa, compared to ABS at 66.13 MPa and PLA at 58.56 MPa. For compression strength, the rHDPE + 10%GP specimens had an average of 22.52 MPa, while ABS and PLA averaged 81.31 MPa and 37.10 MPa, respectively. Additionally, the surface roughness of the rHDPE + 10%GP specimens was observed to be higher, with an average value of 35.28 μm, compared to ABS at 22.43 μm and PLA at 18.17 μm.
However, the rHDPE + 10%GP specimens displayed lower stiffness coupled with a higher strain at break, indicating remarkable ductility and flexibility. This inherent flexibility opens up avenues for applications where high force resistance is not a primary concern, such as in acoustic applications where the ability to absorb sound can be advantageous. A sound absorption test was further carried out to confirm the potential of rHDPE + 10%GP for acoustic applications. The result demonstrated that the rHDPE + 10%GP lattice specimens surpassed both ABS and PLA in terms of absorption coefficient. Specifically, while PLA exhibited a maximum absorption coefficient of 0.64 at 5360 Hz and ABS peaked at 0.68 at 5200 Hz, the rHDPE + 10%GP reached its highest absorption coefficient of 0.76 at 4830 Hz. Importantly, the rHDPE + 10%GP consistently outperformed ABS and PLA, especially within the frequency range of 2160 Hz to 5220 Hz, although its performance tapered off at frequencies exceeding 5450 Hz. This finding underscores the potential of recycled materials like HDPE for use in acoustic applications. Moreover, the sustainability aspect of rHDPE cannot be overlooked. Life cycle analysis comparing recycling with common disposal methods such as landfilling and incineration revealed that recycling significantly reduces pollution levels, global warming impact, and ozone formation.
While rHDPE may not match the mechanical strength of some virgin filaments in printing products, its versatility, flexibility, and sustainability make it a valuable material for diverse applications. As technology evolves and research progresses, we anticipate further enhancements in the quality and performance of recycled materials for 3D printing. Embracing recycled materials not only fosters sustainability but also paves the way for innovation and creativity in 3D printing applications.