Extrusion 3D Printing Processes and Performance Evaluation of GelMA/LPN/MC Hydrogel

doi:10.3901/JME.2022.09.283

Abstract

Abstract: Extrusion 3D printing hydrogels for tissue repair is a research hotspot in recent years. However, the high-fidelity hydrogel printing process is still inseparable from the complex cross-linking strategy, which greatly increases the difficulty of printing and limits the application of hydrogel in the field of tissue engineering. A hydrogel that can be printed at room temperature is prepared, and high-fidelity printing can be achieved without any auxiliary cross-linking during the printing process. The hydrogel is composed of gelatin methacrylate (GelMA), Laponite (LPN) and methylcellulose (MC).The extrusion test screened out the proportion of composite materials suitable for printing, and the process test investigated the effects of extrusion speed and nozzle movement speed on the continuity of the filament and the line width of the microfilament. When the inner diameter of the nozzle is 400 μm, the conditions for GelMA/LPN/MC hydrogel to achieve smooth silk-out (φ400-600 μm) are the extrusion speed of 8.6-13 mm/h and the printing speed of 6-10 mm/s. Rheological results show that the addition of LPN and MC grants the material excellent shear-thinning properties, enabling it to print at room temperature and maintain a stable structure. The compression test shows that changing the crosslinking time can increase the compressive modulus of the composite hydrogel by 5 times and the compressive strength by 3 times. Cell test showed that GelMA/LPN/MC hydrogel has good biocompatibility.

Key words: GelMA, hydrogel, 3D extrusion-based printing, process parameter

CLC Number:

TG156

DONG Lanlan, LI Gen, XIONG Yinze, ZHANG Hang, WANG Lei, LI Xiang. Extrusion 3D Printing Processes and Performance Evaluation of GelMA/LPN/MC Hydrogel[J]. Journal of Mechanical Engineering, 2022, 58(9): 283-290.

References

[1] NORIOKA C, INAMOTO Y, HAJIME C, et al. A universal method to easily design tough and stretchable hydrogels[J]. NPG Asia Materials, 2021, 13(1): 34.
[2] BAHCECIOGLU G, HASIRCI N, BILGEN B, et al. A 3D printed PCL/hydrogel construct with zone-specific biochemical composition mimicking that of the meniscus[J]. Biofabrication, 2019, 11(2): 025002.
[3] WANG C, WANG M, XIA K, et al. A bioactive injectable self-healing anti-inflammatory hydrogel with ultralong extracellular vesicles release synergistically enhances motor functional recovery of spinal cord injury[J]. Bioactive Materials, 2021, 6(8): 2523-34.
[4] YANG J, LIU Y, HE L, et al. Icariin conjugated hyaluronic acid/collagen hydrogel for osteochondral interface restoration[J]. Acta Biomater, 2018, 74: 156-67.
[5] MAO Wei, LIAN Qin, LI Dichen, et al. 3D printing process for hydro gel with the three-dimensional micro tubes to mimic vascular network[J]. Journal of Mechanical Engineering, 2017, 53(9): 180-186. 毛伟, 连芩, 李涤尘, 等. 立体空心血管网水凝胶支架的3D打印工艺研究[J]. 机械工程学报, 2017, 53(9): 180-186.
[6] LI H, TAN C, LI L. Review of 3D printable hydrogels and constructs[J]. Materials & Design, 2018, 159: 20-38.
[7] HEINRICH M A, LIU W, JIMENEZ A, et al. 3D bioprinting: From benches to translational applications[J]. Small, 2019, 15(23): 1805510.
[8] PAXTON N, SMOLAN W, BÖCK T, et al. Proposal to assess printability of bioinks for extrusion-based bioprinting and evaluation of rheological properties governing bioprintability[J]. Biofabrication, 2017, 9(4): 044107.
[9] LEVATO R, JUNGST T, SCHEURING R, et al. From shape to function: The next step in bioprinting[J]. Advanced Materials, 2020, 32: 1906423.
[10] LEI S, GAO Q, ZHAO H, et al. Fiber-based mini tissue with morphology-controllable gelma microfibers[J]. Small, 2018, 14: 1802187.
[11] YIN J, YAN M, WANG Y, et al. 3D bioprinting of low-concentration cell-laden gelatin methacrylate (GelMA) bioinks with a two-step cross-linking strategy[J]. ACS Applied Materials & Interfaces, 2018, 10(8): 6849-6857.
[12] FOYT D, NORMAN M, YU T, et al. Exploiting advanced hydrogel technologies to address key challenges in regenerative medicine[J]. Advanced Healthcare Materials, 2018, 7(8): 1700939.
[13] GU Heng, LIAN Qin, WANG Huichao, et al. Extrusion 3D printing processes and performance evaluation of GelMA composite hydrogel[J]. Journal of Mechanical Engineering, 2020, 56(1): 196-204. 顾恒, 连芩, 王慧超, 等. GelMA复合凝胶的挤出式3D打印工艺及其性能研究[J]. 机械工程学报, 2020, 56(1): 196-204.
[14] OUYANG L, HIGHLEY C B, SUN W, et al. A generalizable strategy for the 3D bioprinting of hydrogels from nonviscous photo-crosslinkable inks[J]. Advanced Materials, 2017, 29(8): 1604983.
[15] SAMIMI GHARAIE S, DABIRI S, AKBARI M. Smart shear-thinning hydrogels as injectable drug delivery systems[J]. Polymers, 2018, 10: 1317.
[16] QUINT J P, MOSTAFAVI A, ENDO Y, et al. In vivo printing of nanoenabled scaffolds for the treatment of skeletal muscle injuries[J]. Advanced Healthcare Materials, 2021, 10(10): 2002152.
[17] GAO Q, NIU X F, SHAO L, et al. 3D printing of complex GelMA-based scaffolds with nanoclay[J]. Biofabrication, 2019, 11(3): 10.
[18] CARRELLA A, BRENNAN M J, WATERS T P. Static analysis of a passive vibration isolator with quasi-zero-stiffness characteristic[J]. Journal of Sound and Vibration, 2007, 301(3): 678-689.
[19] CIDONIO G, ALCALA-OROZCO C R, LIM K S, et al. Osteogenic and angiogenic tissue formation in high fidelity nanocomposite Laponite-gelatin bioinks[J]. Biofabrication, 2019, 11(3): 17.
[20] SHIRAHAMA H, LEE B H, TAN L P, et al. Precise tuning of facile one-pot gelatin methacryloyl (GelMA) synthesis[J]. Scientific Reports, 2016, 6(1): 31036.
[21] WU D, YU Y, TAN J, et al. 3D bioprinting of gellan gum and poly (ethylene glycol) diacrylate based hydrogels to produce human-scale constructs with high-fidelity[J]. Materials & Design, 2018, 160: 486-495.
[22] ZHU F, CHENG L, YIN J, et al. 3D printing of ultratough polyion complex hydrogels[J]. ACS Applied Materials & Interfaces, 2016, 8(45): 31304-10.
[23] LEE B H, LUM N, SEOW L Y, et al. Synthesis and characterization of types A and B gelatin methacryloyl for bioink applications[J]. Materials, 2016, 9(10): 797.
[24] HUANG L, ZHU Z, WU D, et al. Antibacterial poly (ethylene glycol) diacrylate/chitosan hydrogels enhance mechanical adhesiveness and promote skin regeneration[J]. Carbohydrate Polymers, 2019, 225: 115110.