Abstract
In the past two decades, polyether ether ketone (PEEK) has been vastly used in different industries such as automotive, aerospace, and medical sectors due to its mechanical strength, high heat stability, and excellent chemical resistance. Since this semi-crystalline polymer has a high melting temperature, the standard procedure to select extrusion-based 3D printing working parameters has many challenges to ensure each bespoke product with the best quality. Slight shift from optimum process parameters in fused deposition modeling (FDM) of PEEK has a remarkable impact on the final product quality. The present research addresses the long-standing problem of selecting a working setup quickly and accurately which is not dependent on the user's knowledge. In this article, to identify the best arrangement of FDM process parameters, an orthogonal matrix of Taguchi Design of Experiments (DoEs) is applied. Different values of bed, chamber, and nozzle temperatures, print speed, and layer thickness were thoroughly examined for the printing of standard tensile specimens. The mechanical properties and the fracture morphology of samples are examined in different printing conditions to explore a roadmap tool for designing better process parameters which satisfy mechanical requirements of products. In this study, the interpretation of the experimental results is investigated based on analysis of variance (ANOVA). The obtained results show that the best working set up for nozzle temperature, bed temperature, print speed, and layer thickness are 415°C, 160°C, 50 mm s−1, and 0.2 mm, respectively. This article consists of five sections. After introduction in the first section, the effects of working parameters on the strength of final fused products are investigated in Experimental setup section. The results and the confirmation test are considered in seperate sections, respectively. The research is summarized in the conclusion section.
Introduction
In recent years, the 3D printing market has recorded an upward trend in production of components in aerospace, automotive industries, biomedical, and energy sectors along with increasing attention for personalized equipment. 1 Fused deposition modeling (FDM) or fused filament fabrication (FFF) is a widespread process in additive manufacturing (AM) technologies. Low initial investment in equipment and material with high safety and comfort use of filament are the main advantages of FDM. Although acrylonitrile butadiene styrene (ABS), poly lactic acid (PLA), and nylon are the most common filaments for FDM, polyaryletherketone (PAEK) and polyether ether ketone (PEEK) are highly requested recently for FFF technique. 2 PAEK and PEEK are a family of semi-crystalline thermoplastics which have attractive attributes such as high-temperature stability and high mechanical strength. PEEK's biocompatibility, resistance to chemical damage, compatibility with different reinforcing agents (such as glass and carbon fibers), and radiolucency make PEEK a suitable biomaterial for orthopedic, spine and dental implants.3–13 In recent years, the limitations and challenges in 3D printing of PEEK through the FDM process has been the scope of many researchers. Some prevalent problems would occur in PEEK 3D printing such as weak interlayer bonding, distortion of initial layers, delamination, internal pores, high porosity, and internal crack propagation.14–16
Although there are some parameters with tight tolerance that have no impact on the final printing sample, there are some important parameters which can directly affect the mechanical strength and the perfection of PEEK printed products. The best selection of working parameters could improve the print condition and eliminate the probable defects. The effective parameters include print speed, nozzle, bed and chamber temperatures, layer thickness, infill type, infill density, nozzle diameter, PEEK filament quality, desiccation of initial PEEK filament, and post heat treatment. 14 Figure 1 shows the classification of effective parameters in PEEK extrusion-based 3D printing. Nozzle diameter and PEEK filament quality are not adjustable parameters in the FDM process and the engineer should change the hardware of the machine to implement a new setup. The feedstock, filament moisture level, and post heat treatment are also obvious that they cannot be considered as adjustable parameters. The rest of parameters are working setup which can be changed during the print process.

Classification of effective parameters in fused deposition modeling (FDM) of polyether ether ketone (PEEK).
Many studies present the complication of selecting process parameters for printing PEEK specimens. Vaezi and Yang 17 published the first report on successful PEEK 3D printing through FDM process. Rahman et al. 18 investigated the effect of print's raster angle on the mechanical strength. Three raster directions were considered in their experiments, namely 0° (longitudinal), 90° (perpendicular), and 0°/90° alternating. They tested samples thoroughly with uniaxial, tension, flexural, compression, and impact tests. Their results revealed that printing in longitudinal direction presents higher mechanical strength. Zhao et al. 15 run a set of experiments and assessment of mechanical loading tests under different printing conditions such as raster angle (0°, 45°, and 90°), post-treatment along with nozzle and ambient temperatures. Their study investigated individually for finding the best mechanical strength for each parameter to produce high strength biocompatible PEEK scaffold cranial structure. Wang et al. 16 applied a finite element analysis (FEA) and experimental setup simultaneously to investigate the effect of various printing parameters such as nozzle diameter, printing temperature, print speed, printing layer thickness on the mechanical properties, and surface quality of FDM printed parts. Geng et al. 19 studied the effects of the extrusion and printing speeds on the microstructure and dimensions of an extruded PEEK filament. Wang et al. 20 studied the effects of different process parameters such as temperatures of nozzle and plate, printing speed, and layer thickness on the mechanical strength. Song et al. 21 considered the effects of variable process parameters on the porosity and mechanical strength of PEEK. Deng et al. 22 have conducted an experimental research on the effects of PEEK printing parameters such as nozzle temperature, infill speed, and layer thickness on tensile strength. Although there are several research in the literature to investigate the impact of FDM process parameters on mechanical strength, most of them have considered the effect of relevant parameters partially while assuming some items as constant variables. Also, some other researchers did not apply a commercial FDM machine and they could not consider the whole range of all parameters. In this article, the process parameters of fused filament printing including print speed, nozzle temperature, bed temperature, and layer thickness are thoroughly investigated. Three samples per each experimental setup are fabricated and tested for eliminating the stochastic effects on results. The comprehensive data are collected to provide a new guideline to enhance the quality of PEEK products and reduce the fabrication failures. The article is organized as follows: in Experimental setup section, the domain of process parameters is described in detail. The experimental setup is explained in Results and discussion section, followed by morphology observation of the fracture section and in the next section, the confirmation test is done.
Experimental setup
Domain of process parameters
The next step after determining the effective process parameters is to find the best working range of each parameter. Many papers published to consider the effects of process parameters on mechanical strength.14–39 Table 1 summarizes the process parameters domains in the literature for the highest mechanical strength. The common mechanical tests to analyze mechanical strength are tensile, bending, impact, and compressive tests. In the present article the uniaxial tension test has been applied for mechanical strength.
The proposed process parameters.
Selection of working parameters
Ambient or chamber temperature has a key effect on mechanical properties of printed PEEK products. Increasing the chamber temperature improves the print condition. By considering the melting point of PEEK (343°C), increasing the chamber temperature close to melting point makes a lower cooling rate that finally results in high strength samples. The printed components at relatively low chamber temperature will have inappropriate interlayered bonding that creates delamination on the fracture surface 15 while with the increase of the chamber temperature, the delamination is clearly inhibited. Zhao et al. 15 reported that at a temperature higher than 80°C, improvement of the interlayered bonding eliminates the delamination. In the present study, due to the 3D printing machine setup, it is impossible to consider a higher ambient temperature of 90°C and the maximum chamber temperature is fixed to 90oC. Furthermore, the infill type parameter is not considered in present study and all samples are printed in zigzag type. The effective parameters studied in this research are nozzle temperature, bed or platform temperature, feed rate, and layer thickness.
Design of experiments (DoEs) using Taguchi method
It is necessary to carefully design the experimental workflow. In the present study, 4 parameters are considered with 3 levels each, at least 81 experiments (i.e. 34) need to be run for understanding the effects of each variable. Moreover, repetitive tests are needed for elimination of experimental error. In fact, if three sets of repetitive samples are used without implementation of Taguchi method the total experiments reach to 243 states that make the experimental activities time-consuming and costly.
Taguchi technique is an effective tool for the DoEs which reduces the number of required experiments while retaining the impact of each variable on the final output. The steps of Taguchi design are shown in Figure 2.40–51 After running experimental tests, signal-to-noise ratio (SNR) and analysis of variance (ANOVA) were applied to analyze the experimental results. Process parameters for experiments are nozzle temperature (A), bed temperature (B), print speed (C), and layer thickness (D) with three levels of nozzle temperature and two levels of the rest parameters. The selected levels were obtained according to the literature and 3D printing machine limitations. The number of experiments is determined by the orthogonal array (OA) which is the minimum possible matrix for combination of design parameters. In the present study, the total degree of freedom (DOF) is five which should be smaller or at maximum equal to an OA's DOF. Therefore, a Taguchi L8 OA was applied with 7 DOFs. Table 2 shows the L8 OA design to improve experimental efficiency.

The work flow of investigation.
L8 orthogonal array (OA) design for process parameters of polyether ether ketone (PEEK).
FDM machine and material
The specimens are printed using a commercially available 3D printer namely 3DGence INDUSTRY F340. The FIRE WIRE®PEEK filament with average diameter of 1.75 mm and density of 1.29 g cm−3 (manufactured by 3DXTECH, USA) is used as the feed stock.
Samples preparation
The CAD model of the tensile test was created in CATIA V5. The slicer software 3DGence Slicer 4.0 is used to slice the STL file. Eight dumbbell-shaped specimens with 50% infill density (filling ratio) for uniaxial tension test were printed based on standard test method for tensile properties of plastic (D638-14 type IV). 52 To eliminate the interference of experimental error, increase the precision and gaining higher reliability three repetitive samples were printed with the same process parameters.
Porosity evaluation
Each specimen is fully investigated in terms of porosity. The porosity is measured by the following relation.
17
Uniaxial tension test
A fully computerized universal testing machine STM-250 (SANTAM Engineering Design Co. Ltd) with servo electromechanical operation is used for tension test. Testing speed for all samples were fixed at 3.9 mm min−1 that is equivalent to strain rate of 10−3S−1 based on standard test method for tensile properties of plastic (D638-14 type IV). 52
Results and discussion
Tensile test
It is worth to note that for each combination of process parameter, three specimens are printed and the mean value is calculated. Table 3 demonstrates the average tensile strength, the SD for three repetitive samples, elastic modulus, elongation, and average porosity for the proposed experiment. In Table 3m the maximum tensile strength is 44.2 MPa.
Tensile properties of L8 orthogonal array (OA) design.
SNR: signal-to-noise ratio.
SNR and ANOVA
In the Taguchi approach, SNR measures the effect of design parameters on the final output. The three models of SNR are used for Taguchi are (a) nominal is better (to achieve the target with minimum deviation), (b) larger is better (to maximize the response), and (c) smaller is better (to minimize the response). 40
In the present study, the design parameters are process parameters, the final output is tensile strength, and the objective is selected to be the best selection of input parameters which provides the highest tensile strength. The second type of SNR expressed by equation (2) was applied.

The main effects plot for signal-to-noise (SNR).
The interactions between different parameters are not considered in this study. In Table 4, range analysis of L8 orthogonal experiments is listed. In equation (3), Kij (i = 1, 2, 3) is the sum of experimental results in terms of level i, kij the mean of Kij, and R represents the range.
Range analysis of tensile strength.
According to the order of priority (ABDC), the nozzle temperature has the highest impact on the tensile strength. Although the impact order of process parameters can be detected in the analysis, the influence of each parameter individually is a challenging subject. 40
ANOVA as a statistical technique was applied to interpret the experimental data and complementary analysis. ANOVA results are shown in Table 5 with two important parameters F and P, which indicate variance ratio and percent of contribution, respectively. F-value is a ratio of the mean of squared deviations to the mean of squared errors and p-value is the percentage contribution of each parameter.
40
These values could be determined directly using equations (4) and (5).
Analysis of variance (ANOVA) result for tensile strength.
In equaiton (4),
Influence of process parameters on tensile property
Nozzle and bed temperatures
The nozzle temperature has the most effectiveness (42%) on tensile strength. Figure 4 indicates the mean experimental results in nozzle temperature of 390, 415, and 430°C. The nozzle heat has the direct effect on adhesion of layers. The higher temperature of extruded material provides better adhesion to the previous printed layer which is a solid state. Furthermore, the low viscosity and high fluidity at high temperature leads to being well printed without blocking the nozzle. 35 Higher temperature transfers more energy to PEEK filament so the internal microvoids decrease and the strength of specimens would increase. On the other side, higher printed temperature creates better crystallization because the longer time would be allocated between the printed temperature and the ambient temperature.21,23

Tensile strength for different levels of nozzle temperature (a) and bed's temperature (b).
Figure 5(a) and (b) show the comparison between the specimen No. 1 from L8 OA which is printed in 390°C as the worst experiment (the lowest tensile strength) and the specimen No. 7 which is printed in 415°C as the best one (the highest tensile strength). Figure 5(b) indicates the appropriate filament-to-filament and interlayer bonding and inversely Figure 5(a) shows the weak bonding. Figure 5(b) indicates regular and proper bonding of sequence layers.

Microstructure of fracture surface. (a) Specimen No. 1 (390°C), (b) specimen No. 7 (415°C), and (c) specimen No. 8 (440°C).
Figure 6 focuses on fusion line between infill filaments. In Figure 6(b), the layer connectivity shows good fusion for specimen No. 7 compare to Figure 6(a) which is related to specimen No. 1. The uniform wire fusion is clear during the FDM process. Based on Figure 6, the lower print speed and lower temperature lead to un-uniform deposition. 22 Although the high nozzle temperature leads to better adhesion, the excessive heating can make it worse. Finding an optimum temperature is not straightforward and depends on each case. The optimum value of nozzle temperature is 415°C. In fact, the increase in the nozzle temperature than optimum value leads to the decrease in the strength (Figure 4). The specimen No. 8 with highest selected temperature of 440°C has created lower tensile strength. Based on Table 4, the A3 (mean strength of specimens which is printed in 440°C) amount of 4.1 MPa is the lower compared to A2 (mean strength of specimens which is printed in 415°C).

Representative scanning electron micrographs of fracture surfaces. (a) Specimen No. 1 (390°C) and (b) specimen No. 7 (415°C).
With the increase of nozzle temperature than optimum value, three prevalent issues will happen. First, the diluted deposited filament with high energy has a deep penetrative effect. Each layer might be affected several times during printing the top layers and therefore, the solidification process is not uniform. Figure 5(c) represents the micrographs of fracture surface for specimen No. 8 with 440°C. Layers crush on each other in white rectangles in Figure 5(c) compared to Figure 5(b) which indicates regular bonding between layers. In Figure 5(b), layers are formed disorderly. Second, the degradation of PEEK will produce gas which will emerge in the deposited layer as micropores. The layer pores are shown in Figure 7. Micropores in the layer are resulted of the entrapped gases. They are generated by excessive heating from optimum temperature. Higher temperature will affect the volume and numbers of these micropores. When the porosity increases, the strength of the specimen will decrease. At micrographs of present experiments, this type of pore was not observed (it might emerge at higher temperatures). Third, low viscosity of melted filament does not create a whole defined thickness. Therefore, the distance between printed layers will occur. The next layer will print with air gaps between layers. The interlayer pores in Figure 7 demonstrate these gaps schematically between deposited layers.

The layer pores and interlayer pores in fused deposition modeling (FDM) at higher temperatures than optimum value.
The nozzle temperature directly determines the viscosity of melted filament which plays an important role in the form of structure. While the appropriate viscosity of deposited filament creates a proper thickness and, the next layer is deposited uniformly without any gap, and extra dilution of melted filament cannot create a proper and entire thickness. Figure 8(a) and (b) show two adjacent layers of specimen No. 7 with 415°C and specimen No. 8 with 440°C, respectively.

The observation of interlayer micropores. (a) Specimen No. 7 (415°C) and (b) specimen No. 8 (440°C).
The interlayer pores are specified with red rectangle in Figure 8(b). Un-uniform surfaces along with distance and gaps between two subsequent printed layers make high porosity which can decrease the strength of samples. According to the order of priority in Table 4 (ABDC), the second priority is the bed temperature with a p-value of 24%. The higher bed temperature provides higher adhesion. At constant low chamber temperature of the present experiment (90°C), higher temperature of bed or platform plays an important role in warming up the initial layers which are adjacent to the bed. Figure 4 shows the mean experimental results in bed temperature. If the limitation of 3D printer machine, allows the chamber temperature to increase up to 250°C (such as Wang et al. 14 ), the bed temperature will shift from the second priority to the lower importance.
Print speed and layer thickness
The third and fourth priorities are layer thickness and print speed, respectively. Figure 9 shows the tensile strength for different levels of these factors.

Tensile strength for different levels of layer thickness and print speed.
Although increasing the layer thickness provides low surface quality, 14 thick layer has more preservation of heat and creates low cooling rate, and therefore, the subsequent layer takes higher adhesion. More preservation of heat will happen at a fast speed for merging the two adjacent layers. On the other side, when PEEK prints quickly, the material does not have sufficient time to form and orient. Weak bonding strength between the two adjacent printing layers will occur at the downside of rapid printing. The obtained experimental results indicate that the effect of heat preservation overcomes the orientation factor. The higher print speed leads to a higher strength specimen.
Confirmation test
The final step is to predict the best value for each parameter based on Taguchi approach and ANOVA in order to improve the tensile strength. According to the range analysis of tensile strength based on Taguchi results, the optimum combination is A2B2C2D2. Considering Taguchi approach, the best value for optimum combination is calculated. The maximum estimated tensile strength of Taguchi (Tmax) is calculated by

Stress–strain curves of optimum L8 combination and new optimized experiment.
Conclusion
In the present study, the uniaxial tension test of PEEK samples at different FDM printing conditions is thoroughly studied. The basic parameters which have major effect on mechanical strength are listed and the domain of each parameter and the best value of them are indicated. Nozzle temperature, print speed, platform temperature, and layer thickness were considered as the effective parameters for PEEK printing. Based on Taguchi, an L8 OA was applied in the experiments. The levels for nozzle temperature are selected in three different levels including 390°C, 415°C, and 440°C. Experiments revealed that the best value for nozzle temperature is 415°C, whereas lower values provide weak bonding connectivity and higher temperature provides disordered layer adhesion. The SEM microstructures of specimens with different nozzle temperatures were compared. The levels of platform temperature were selected 120°C and 160°C. The levels of print speed were selected as 10 mm s−1 and 50 mm s−1. The levels of layer thickness were selected as 0.1 mm and 0.2 mm. Based on L8 Taguchi result, the best value for platform temperature, print speed, and layer thickness are 160°C, 50 mm s−1, and 0.2 mm, respectively. By applying range analysis for Taguchi, the best estimated process parameter was calculated. A new specimen with calculated process parameter was fabricated and then was tested experimentally. The comparison of Taguchi optimum condition and the new fabricated test demonstrated a good agreement.
Footnotes
Declaration of conflicting interests
The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.
Funding
The authors acknowledge the funding support of Babol Noshirvani University of Technology through Grant program No BNUT/370434/01.
