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The die swell eliminating mechanism of hot air assisted 3D printing of GF/PP and its influence on the product performance

  • Ru Yang , Jianhua Xiao EMAIL logo , YingLan Liu and ShiKang Xu
Published/Copyright: March 16, 2024
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e-Polymers
From the journal e-Polymers Volume 24 Issue 1

Abstract

For eliminating the die swell phenomenon in 3D printing of GF/PP, a hot air assisted 3D printing method is proposed and its mechanism is studied. A two-phase flow model consisting of compressible gas and in-compressible melt is established, and the process of polymer filament extrusion is simulated. A series of experiments are conducted to compare the differences between traditional printing and gas-assisted printing in terms of extruded filament, temperature, and morphology. The simulation and experiment results show that the addition of gas effectively mitigates the melt die swell, and increases the extrusion filament temperature to more than 70°C. The extrusion pressure is reduced about two orders of magnitude, and the first normal stress is decreased from 400,000 to 20,000 Pa. The surface morphology of printed product is smoother and more refined. This study provides valuable information for understanding the principles of gas-assisted printing and demonstrates its potential for improving printing quality and efficiency.

Keywords: additive manufacturing; fused deposition modeling; gas-assisted; hot air; die swell

1 Introduction

Fused deposition molding (FDM) is a low-cost and high-efficiency 3D printing technology (1). It extrudes thermoplastic polymer filaments through a nozzle and deposits on a support platform layer by layer (2). This technology has been widely used in medical, aerospace, and industrial applications (3). However, FDM still has some limitations, such as high roughness (4), low accuracy, poor bonding strength between layers, and easy cracking (5).

In order to solve these problems, Nomani et al. (6) studied the effect of layer thickness on the mechanical properties of the products and found that smaller layer thicknesses result in the stronger and stiffer products. Chithambaram and Senthilnathan (7) studied the relationship between printing parameters and surface roughness of PEEK. They found that the lowest surface roughness of the samples is obtained at a layer height of 0.15 mm and a printing speed of 20 mm·s−1. Marius et al. (8) printed carbon fiber impregnated PLA and found that the pore volume of the product decreases while the tensile strength increases with the decrease in layer thickness and line width. Anant et al. (9) studied the effect of layer thicknesses, filling modes, and filling densities on the mechanical properties of 3D printed ABS materials. They found that the tensile and impact strengths are substantially improved with minimum layer thickness, filling density, and concentric filling mode. Austin et al. (10) found that the off-film die swell effect increases with the increase in the volumetric flow rate and shear stress, and decreases with the increase in the hot end temperature and nozzle orifice diameter. Geng et al. (11) also found that higher heat treatment temperatures improve tensile strength and fracture toughness. Ravoori et al. (12) heated the deposited layer with a hot metal block and measured the temperature with an infrared camera. It showed that the temperature of the deposited filaments was significantly increased, which helps in the adhesion of the printed filaments. Prajapati et al. (13) added a hot air heating block onto the print head, which increases the strength and toughness of the prints and improved the quality of the prints. Serdeczny et al. (14) performed numerical simulations of polymer flow inside the nozzle in FDM to explain the pressure and melt zone oscillations that occur during unsteady extrusion. They found that a circulation zone is formed between the feed filament and the die wall, which prevents excessive polymer reflux and clogging of the feed mechanism.

Xu et al. (15) introduced gas-assisted technology into FDM by installing special gas-assisted printing nozzles in 3D printers. The high-temperature and high-pressure gas streams form a thin layer of gas between the metal nozzles and polymer filaments. This gas layer reduces the friction between the mold and the melt, allowing the FDM filament to be extruded in a completely slippery manner. This technique eliminates extrusion bloom, resulting in smooth surfaces and good-quality 3D-printed products. In its experiments, the unidirectional gas inlet cannot reveal the specific mechanism of the gas on the printed filament, in order to study this problem in depth, this work improves the gas-assisted printing nozzle, and uses numerical simulation methods to simulate the convergence of the gas, the melt in the mold, and the whole process of extrusion. By comparing the difference between gas-assisted 3D printing and traditional 3D printing, the feasibility of gas-assisted printing technology is verified.

2 Experimental set up

Glass fiber reinforced polypropylene used in this experiment is EP015606BK001 with 10% glass fiber filling produced by Hangzhou Jufeng New Materials Co., Ltd.

The 3D printer selected for this experiment is DK280 produced by Shenzhen Dakun Additive Manufacturing Co., Ltd. The gas heater selected for this experiment is 17-3-8005 produced by Shanghai Laiheng Electric Heating Appliance Co., Ltd. The Microprocessor controlled electronic selected for this experiment is UTM4203 produced by Shenzhen Sansi Zongheng Technology Co., Ltd. The confocal microscope selected for this experiment is CHOTEST-VT6000 produced by Shenzhen Zhongtu Instrument Co., Ltd. The thermal imager selected for this experiment is FLIR E54 produced by Philips Technologies.

3D printing parameters and gas-assisted 3D printing parameters are listed separately in Tables 1 and 2.

Table 1

3D printing parameters of GF/PP materials

3D printing Parameter 3D printing Parameter
Nozzle temperature (°C) 240 Bed temperature (°C) 0
Layer thickness (mm) 0.1 Printing speed (mm·s−1) 30
Deposit orientation (°) 0/90 File diameter (mm) 1.75
Filling rate (%) 100 Nozzle diameter (mm) 1.0
Table 2

Gas-assisted 3D printing parameters of GF/PP materials

Gas-assisted 3D printing Parameter
Gas temperature (°C) 240
Gas pressure (MPa) 0.15
Gas flow rate (L·min−1) 1.5
Nozzle diameter (mm) 1.0

The gas-assisted experimental setup is shown in Figures 1 and 2.

Figure 1 Schematic diagram of the experimental system.
Figure 1

Schematic diagram of the experimental system.

Figure 2 (a) Gas-assisted 3D printing nozzle; (b) gas-assisted 3D printer.
Figure 2

(a) Gas-assisted 3D printing nozzle; (b) gas-assisted 3D printer.

As shown in Figure 1, an experimental system for gas-assisted printing is established in this study. It consists of an air compressor, a gas regulating valve, a gas flow meter, a gas heater, and a 3D printer. The gas-assisted nozzle (Figure 2a), refined from the traditional 3D printing nozzle, has an additional gas channel. Gas via the inlet channel located at the top surface of heat block enters into a circular gas chamber, and then enters into the throat. Meantime, the GF/PP filament passes through the guide tube and enters the throat. In the throat a circular gas film around GF/PP melt is formed and enter into the nozzle with the melt. Due to the angle between gas and filament at the confluence, normal forces will decompose, directly affecting the surface fracture of filament after extrusion, so the inner wall of the gas nozzle is designed as shape of streamlined. The stability of gas transportation, the rationality of assembly, and the compactness of the nozzle unit structure have been considered in the designing.

3 Numerical modeling

3.1 Geometric models and finite element models

The profile of the gas-assisted printing nozzle designed in the experiment is shown in Figure 3a. A 2D 1/2 symmetric geometric model used in this numerical simulation is established and shown in Figure 3b. There are inner and outer domains in the models: inner domain represents melt extrusion, and outer domain represents gas layer. The radius of the melt in this model is 0.4 mm, and the thickness of gas layer is 0.1 mm. The length inside and outside the nozzle are both 3 mm.

Figure 3 Gas-assisted printing nozzle cross-section with details.
Figure 3

Gas-assisted printing nozzle cross-section with details.

According to the flow characteristics of polymer melt and gas in gas-assisted extrusion, the following assumptions are made for numerical simulation: the gas is a compressible fluid, and the polymer melt is an in-compressible viscoelasticity fluid; the effects of inertial and gravitational forces on the two types of fluids are neglected; the friction and viscous heating are neglected; and the effects of relative slip, interpenetration, and surface tension between the gas and melt are neglected.

Based on the above assumptions, the continuity equation, the momentum conservation equation, the energy conservation equation, the PTT equation which can well describe the polymer morphology, and the intrinsic equation of the gas are used in the simulation.

(1) exp ε λ ( 1 − η r ) η tr ( τ 1 ) + λ 1 − ξ 2 ∇ τ 1 + ξ 2 ∆ τ 1 = 2 ( 1 − η r ) η 1 D

(2) τ = τ 1 + τ 2

(3) τ 2 = 2 η 2 D

(4) η r = η 2 η

where τ is the melt stress tensor, τ 1 is the elastic component in the deviatoric stress tensor, τ 2 is the pure viscous tensor in the deviatoric stress tensor, η 1 is the total viscosity of the melt, η 2 is the Newtonian viscosity of the melt, η r = η r/η 1 is the viscosity ratio, λ is the relaxation time of the polymer melt, ε is the material parameter related to the tensile properties of the polymer melt, ξ is the material parameter related to the shear viscosity of the polymer melt, and D is the deformation rate tensor.

For gases, the constitutive equation is as follows:

(5) τ 1 = 2 η 1 D 1

where η 1 is the viscosity of the gas, and D 1 is the strain rate tensor of the gas.

The physical parameters of the polymer and the air used in the simulation are as shown in Table 3. The melt flow rate is set to 1.0 mm3·s−1 and the gas flow rate is set to 2.4 × 104 mm3·s−1. Both the temperature of melt and gas are 240°C.

Table 3

Physical parameters of polymer melts and gas

Fluid Viscosity (Pa·s) Relaxation time (s) ε ξ s
Melt 8,823 0.1 0.15 0.44 0.12
Gas 2.6 × 10−5 — — — —

3.2 Simulation result

The simulation results of conventional 3D printing and gas-assisted 3D printing are compared in Figure 4.

Figure 4 Extruded melt morphology: (a) traditional 3D printing; (b) gas-assisted printing; and (c) extrusion swelling curves for different printing methods.
Figure 4

Extruded melt morphology: (a) traditional 3D printing; (b) gas-assisted printing; and (c) extrusion swelling curves for different printing methods.

From the figure, it can be seen that the traditional 3D printing has an obvious die swell phenomenon. While under gas-assisted conditions, due to the formation of a more stable gas-assisted lubrication layer in the inner wall of the gas-assisted nozzle, the polymer filament is extruded from stick to slip manner, effectively mitigating the die swell. Due to the gas layer occupying a thin layer of nozzle channel, the extrusion diameter is approximately 97.5% of the nozzle diameter, slightly lower than the nozzle diameter.

The axial velocity of the polymer filament inside the die responds to the motion perpendicular to the extrusion direction. As can be seen from the velocity distribution cloud in Figure 5, conventional traditional printing has the highest normal forward velocity at the nozzle exit, leading to die swell. Conversely, in the gas-assisted printing method, the extruded melt does not undergo die swell due to the action of the gas layer.

Figure 5 R-direction velocity of melt. (a) Traditional 3D printing; and (b) gas-assisted printing.
Figure 5

R-direction velocity of melt. (a) Traditional 3D printing; and (b) gas-assisted printing.

Figure 6 shows the pressure distribution contour of two different printing methods. As can be seen from the figure, traditional printing methods exhibit the highest pressure at the entrance, which gradually decreases linearly along the direction of melt extrusion. This is because in traditional printing extrusion nozzles, the melt experiences high shear rates and shear stresses in the die, increasing the friction between the polymer melt and the die wall, leading to increased pressure at the die. In contrast, gas-assisted extrusion forms a gas layer between the polymer melt and the die, reducing frictional resistance. This transformation from non-slip extrusion to slip extrusion, reduces melt pressure, improving melt extrusion efficiency, and reducing printer energy consumption.

Figure 6 Melt pressure distribution. (a) Traditional 3D printing; and (b) gas-assisted printing.
Figure 6

Melt pressure distribution. (a) Traditional 3D printing; and (b) gas-assisted printing.

The first normal stress difference is an important factor in studying melt extrusion swell. In this article, N 1 = τ yy − τ xx . As can be seen from Figure 7, traditional airless printing produces a large first normal stress difference at the nozzle exit, which makes the filament prone to extrusion swell after extrusion through the nozzle. In contrast, the overall value of the first normal stress difference in gas-assisted printing is relatively small.

Figure 7 Melt stress distribution. (a) Traditional 3D printing and (b) gas-assisted printing.
Figure 7

Melt stress distribution. (a) Traditional 3D printing and (b) gas-assisted printing.

It can be concluded that the presence of a gas layer slows down extrusion swell, resulting in smooth surfaces. In practical printing or extrusion molding, the input of gas should be stabilized as much as possible to improve the stability and quality of printing or extrusion molding.

4 Experimental result

In traditional 3D printing and gas assisted 3D printing, the temperature of the melt and gas is 240°C.

Figure 8a shows the results of traditional extrusion, from which it can be seen that there is an obvious die swell phenomenon. Figure 8b illustrates the outcome of extrusion using the gas-assisted nozzle, revealing a smooth filament surface with uniform diameter, which noticeably mitigates the die swell phenomenon.

Figure 8 Die swell of GF/PP. (a) Traditional 3D printing and (b) gas-assisted printing.
Figure 8

Die swell of GF/PP. (a) Traditional 3D printing and (b) gas-assisted printing.

Figure 9 presents the temperature differences between different printing methods observed by infrared thermography. It can be seen that after the filament is extruded from the print nozzle (Figure 9a, d), the temperature of the extruded filament with gas-assisted printing is higher than the temperature of the conventional extruded filament (Sp3, Sp4, Sp5) (Figure 10). Figure 9c, f show the process of printing the product, which also reflects temperature changes (Figure 9b, e). This temperature difference suggests that the gas-assisted printing technology may provide more heat to the filament during the extrusion process, leading to an increase in its temperature.

Figure 9 Comparison of extruded filament temperature under different printing methods.
Figure 9

Comparison of extruded filament temperature under different printing methods.

Figure 10 (a) Temperature maps at different points of the thermal imager and (b) temperature variation diagram of filament under different printing methods.
Figure 10

(a) Temperature maps at different points of the thermal imager and (b) temperature variation diagram of filament under different printing methods.

This may be due to the additional heating effect on the filament by the high-temperature and high-pressure hot gas stream in gas-assisted printing. This finding provides important insights into our understanding of the thermal behavior of gas-assisted and gas-assist-free printing during processing and may be instructive for optimizing the printing process and improving the quality of printed products. Figure 11 shows the cross-sectional microstructure of gas-assisted printing and traditional printing under different printing directions. It can be proven from the printing in different directions that the filament of gas-assisted printing Figure 11(b) and (d) is more tightly bonded and has fewer pores compared to traditional printing Figure 11(a) and (c). Combined with Figure 9c, it can be clearly seen that the surface quality of the products made by gas-assisted printing technology is superior to that of the products made by gas-assisted printing technology without gas-assisted printing. The surfaces of the gas-assisted printed products appear smoother and flatter, which may be attributed to the uniform pressure and flow of gas during the gas-assisted printing process, which effectively reduces the imperfections and irregularities that may occur during the printing process. In contrast, the surface of the non-gas-assisted printed products may show some minor bumps and irregularities.

Figure 11 Section morphology of printed products under different printing methods.
Figure 11

Section morphology of printed products under different printing methods.

The impact test process is shown in Figure 12, the traditional printing technique exhibited a pronounced cross-sectional discontinuity, whereas the gas-assisted printing specimens demonstrated superior resilience. Under identical experimental conditions, the gas-assisted printed samples remained intact, indicating superior resistance to impact forces. To ensure rigorous evaluation of the impact performance of both printing methods, we conducted five replicate comparative experiments, compiling the findings in Table 4. Through rigorous data analysis, we conclude that gas-assisted printing significantly outperforms traditional printing methods in terms of impact resistance. These observations further confirm the advantages of gas-assisted printing technology in improving the surface quality of printed products and provides a strong basis for choosing a more suitable printing technology in the manufacturing process.

Figure 12 Impact test specimen: (a) Traditional 3D printing and (b) gas-assisted 3D printing.
Figure 12

Impact test specimen: (a) Traditional 3D printing and (b) gas-assisted 3D printing.

Table 4

Impact strength under different printing methods

Different printing methods Impact strength (kJ·m−2)
1 2 3 4 5 Average
Traditional 3D printing 2.18 3.35 2.35 2.20 3.05 2.63
Gas-assisted 3D printing 4.43 4.95 4.00 4.25 4.60 4.45

5 Conclusion

Through a comparison between traditional 3D printing and gas-assisted 3D printing, it becomes evident that gas-assisted 3D printing can basically eliminate die swell and effectively reduce pressure drop inside the nozzle. The research has demonstrated that under gas-assisted conditions, the temperature within the printing process remains more stable, resulting in a product that closely resembles the intended model size. Furthermore, the surface quality is significantly smoother, and the strength is enhanced, exhibiting superior mechanical properties overall.

The simulation results show that the introduction of gas-assisted technology reduces the pressure of the melt, reduces the first normal stress difference, reduces the energy loss of the printer, and eliminates the phenomenon of die swelling. Due to the generation of a certain X reverse velocity at the entrance of the melt, the melt shrinks towards the middle, resulting in a decrease in the diameter of the extruded filament.

In order to improve the quality of 3D printed products, gas-assisted technology can be introduced. In practical operation, to ensure the diameter of the extruded melt, gas related parameters should be reasonably set.

  1. Funding information: This work was supported by the National Natural Science Foundation of China (NSFC) (No. 52063021). Grant Recipient: Jianhua Xiao.

  2. Author contributions: RU yang: writing – original draft, data curation; Jianhua Xiao: writing – review and editing; Yinglan Liu: investigation and supervision; Shikang Xu: investigation and supervision.

  3. Conflict of interest: The authors declare no conflict of interest.

  4. Data availability statement: Not applicable.

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Received: 2024-01-10
Revised: 2024-02-07
Accepted: 2024-02-08
Published Online: 2024-03-16

© 2024 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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https://doi.org/10.1515/epoly-2024-0008
Keywords for this article
additive manufacturing; fused deposition modeling; gas-assisted; hot air; die swell
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  10. Rheological behavior of particle-filled polymer suspensions and its influence on surface structure of the coated electrodes
  11. The effects of property variation on the dripping behaviour of polymers during UL94 test simulated by particle finite element method
  12. Experimental evaluation on compression-after-impact behavior of perforated sandwich panel comprised of foam core and glass fiber reinforced epoxy hybrid facesheets
  13. Synthesis, characterization and evaluation of a pH-responsive molecular imprinted polymer for Matrine as an intelligent drug delivery system
  14. Twist-related parametric optimization of Joule heating-triggered highly stretchable thermochromic wrapped yarns using technique for order preference by similarity to ideal solution
  15. Comparative analysis of flow factors and crystallinity in conventional extrusion and gas-assisted extrusion
  16. Simulation approach to study kinetic heterogeneity of gadolinium catalytic system in the 1,4-cis-polyisoprene production
  17. Properties of kenaf fiber-reinforced polyamide 6 composites
  18. Cellulose acetate filter rods tuned by surface engineering modification for typical smoke components adsorption
  19. A blue fluorescent waterborne polyurethane-based Zn(ii) complex with antibacterial activity
  20. Experimental investigation on damage mechanism of GFRP laminates embedded with/without steel wire mesh under low-velocity-impact and post-impact tensile loading
  21. Preparation and application research of composites with low vacuum outgassing and excellent electromagnetic sealing performance
  22. Assessing the recycling potential of thermosetting polymer waste in high-density polyethylene composites for safety helmet applications
  23. Mesoscale mechanics investigation of multi-component solid propellant systems
  24. Preparation of HTV silicone rubber with hydrophobic–uvioresistant composite coating and the aging research
  25. Experimental investigation on tensile behavior of CFRP bolted joints subjected to hydrothermal aging
  26. Structure and transition behavior of crosslinked poly(2-(2-methoxyethoxy) ethylmethacrylate-co-(ethyleneglycol) methacrylate) gel film on cellulosic-based flat substrate
  27. Mechanical properties and thermal stability of high-temperature (cooking temperature)-resistant PP/HDPE/POE composites
  28. Preparation of itaconic acid-modified epoxy resins and comparative study on the properties of it and epoxy acrylates
  29. Synthesis and properties of novel degradable polyglycolide-based polyurethanes
  30. Fatigue life prediction method of carbon fiber-reinforced composites
  31. Thermal, morphological, and structural characterization of starch-based bio-polymers for melt spinnability
  32. Robust biaxially stretchable polylactic acid films based on the highly oriented chain network and “nano-walls” containing zinc phenylphosphonate and calcium sulfate whisker: Superior mechanical, barrier, and optical properties
  33. ARGET ATRP of styrene with low catalyst usage in bio-based solvent γ-valerolactone
  34. New PMMA-InP/ZnS nanohybrid coatings for improving the performance of c-Si photovoltaic cells
  35. Impacts of the calcinated clay on structure and gamma-ray shielding capacity of epoxy-based composites
  36. Preparation of cardanol-based curing agent for underwater drainage pipeline repairs
  37. Preparation of lightweight PBS foams with high ductility and impact toughness by foam injection molding
  38. Gamma-ray shielding investigation of nano- and microstructures of SnO on polyester resin composites: Experimental and theoretical study
  39. Experimental study on impact and flexural behaviors of CFRP/aluminum-honeycomb sandwich panel
  40. Normal-hexane treatment on PET-based waste fiber depolymerization process
  41. Effect of tannic acid chelating treatment on thermo-oxidative aging property of natural rubber
  42. Design, synthesis, and characterization of novel copolymer gel particles for water-plugging applications
  43. Influence of 1,1′-Azobis(cyclohexanezonitrile) on the thermo-oxidative aging performance of diolefin elastomers
  44. Characteristics of cellulose nanofibril films prepared by liquid- and gas-phase esterification processes
  45. Investigation on the biaxial stretching deformation mechanism of PA6 film based on finite element method
  46. Simultaneous effects of temperature and backbone length on static and dynamic properties of high-density polyethylene-1-butene copolymer melt: Equilibrium molecular dynamics approach
  47. Research on microscopic structure–activity relationship of AP particle–matrix interface in HTPB propellant
  48. Three-layered films enable efficient passive radiation cooling of buildings
  49. Electrospun nanofibers membranes of La(OH)3/PAN as a versatile adsorbent for fluoride remediation: Performance and mechanisms
  50. Preparation and characterization of biodegradable polyester fibers enhanced with antibacterial and antiviral organic composites
  51. Preparation of hydrophobic silicone rubber composite insulators and the research of anti-aging performance
  52. Surface modification of sepiolite and its application in one-component silicone potting adhesive
  53. Study on hydrophobicity and aging characteristics of epoxy resin modified with nano-MgO
  54. Optimization of baffle’s height in an asymmetric twin-screw extruder using the response surface model
  55. Effect of surface treatment of nickel-coated graphite on conductive rubber
  56. Experimental investigation on low-velocity impact and compression after impact behaviors of GFRP laminates with steel mesh reinforced
  57. Development and characterization of acetylated and acetylated surface-modified tapioca starches as a carrier material for linalool
  58. Investigation of the compaction density of electromagnetic moulding of poly(ether-ketone-ketone) polymer powder
  59. Experimental investigation on low-velocity-impact and post-impact-tension behaviors of GFRP T-joints after hydrothermal aging
  60. The repeated low-velocity impact response and damage accumulation of shape memory alloy hybrid composite laminates
  61. Exploring a new method for high-performance TPSiV preparation through innovative Si–H/Pt curing system in VSR/TPU blends
  62. Large-scale production of highly responsive, stretchable, and conductive wrapped yarns for wearable strain sensors
  63. Preparation of natural raw rubber and silica/NR composites with low generation heat through aqueous silane flocculation
  64. Molecular dynamics simulation of the interaction between polybutylene terephthalate and A3 during thermal-oxidative aging
  65. Crashworthiness of GFRP/aluminum hybrid square tubes under quasi-static compression and single/repeated impact
  66. Review Articles
  67. Recent advancements in multinuclear early transition metal catalysts for olefin polymerization through cooperative effects
  68. Impact of ionic liquids on the thermal properties of polymer composites
  69. Recent progress in properties and application of antibacterial food packaging materials based on polyvinyl alcohol
  70. Additive manufacturing (3D printing) technologies for fiber-reinforced polymer composite materials: A review on fabrication methods and process parameters
  71. Rapid Communication
  72. Design, synthesis, characterization, and adsorption capacities of novel superabsorbent polymers derived from poly (potato starch xanthate-graft-acrylamide)
  73. Special Issue: Biodegradable and bio-based polymers: Green approaches (Guest Editors: Kumaran Subramanian, A. Wilson Santhosh Kumar, and Venkatajothi Ramarao)
  74. Development of smart core–shell nanoparticles-based sensors for diagnostics of salivary alpha-amylase in biomedical and forensics
  75. Thermoplastic-polymer matrix composite of banana/betel nut husk fiber reinforcement: Physico-mechanical properties evaluation
  76. Special Issue: Electrospun Functional Materials
  77. Electrospun polyacrylonitrile/regenerated cellulose/citral nanofibers as active food packagings
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