Abstract
Electrospun nanofiber membranes possess high specific surface area with small pores and thus can be developed as wound dressings for absorbing exudate and also preventing bacterial penetration. In this study, hydroxypropyl cellulose (H), chitosan (C) and polyethylene oxide (P) were chosen as membrane materials to increase the hydrophilicity, anti-bacterial property, and yield of nanofibers, respectively. Additionally, graphene (G) was added to enhance the anti-bacterial property of the membranes. As indicated by SEM, the HCP and HCPG solutions (containing H:4.5 wt%, C:4.5 wt%, P:0.75 wt%, without/with G:0.5 wt%) could be electrospun into HCP and HCPG nanofiber membranes with good fiber morphology using a non-toxic solvent system. Further, the membranes were crosslinked by glutaraldehyde vapor to improve the strength. The tensile strength of the membranes was 1.38–1.82 MPa with a swelling ratio up to 1330–1410%. The water vapor transmission rate (WVTR) of wet HCPG membrane was about 3100 g/m2-day, close to the recommended WVTR of wound dressings. The anti-bacterial properties of the membranes were confirmed using three tests against Escherichia coli (Gram-negative bacterium) and Staphylococcus aureus (Gram-positive bacterium). Highly hydrophilic HCP and HCPG membranes prevented the bacterial adherence. The presence of the membranes (especially graphene-embedded HCPG membrane) also greatly reduced bacterial growth. The small pore sizes of HCP and HCPG nanofiber membranes prevented the bacterial penetration to cause infection. Taken together, the HCP and HCPG nanofiber membranes possessed good mechanical properties, appropriate WVTR and high water absorption thus suitable for absorbing wound exudate. Besides, the membranes exhibited nontoxic, anti-fibroblast adhesion and anti-bacterial properties. Therefore, HCP and HCPG nanofiber membranes have the potential to become superior anti-bacterial wound dressings.
Graphic abstract
Similar content being viewed by others
References
Akhavan O, Ghaderi E (2010) Toxicity of graphene and graphene oxide nanowalls against bacteria. ACS Nano 4:5731–5736
Ardila N, Medina N, Arkoun M, Heuzey M-C, Ajji A, Panchal CJ (2016) Chitosan-bacterial nanocellulose nanofibrous structures for potential wound dressing applications. Cellulose 23:3089–3104
Benhabiles MS, Salah R, Lounici H, Drouiche N, Goosen MFA, Mameri N (2012) Antibacterial activity of chitin, chitosan and its oligomers prepared from shrimp shell waste. Food Hydrocoll 29:48–56
Bernardi P, Scorrano L, Colonna R, Petronilli V, Di Lisa F (1999) Mitochondria and cell death. Eur J Biochem 264:687–701
Cao Z, Luo X, Zhang H, Fu Z, Shen Z, Cai N, Xue Y, Yu F (2016) A facile and green strategy for the preparation of porous chitosan-coated cellulose composite membranes for potential applications as wound dressing. Cellulose 23:1349–1361
Chang AKT, Frias RR, Alvarez LV, Bigol UG, Guzman JPMD (2019) Comparative antibacterial activity of commercial chitosan and chitosan extracted from Auricularia sp. Biocatal Agric Biotechnol 17:189–195
Chen PW (2012) Preparation and characterization of multicomponent chitosan composite dressings. Master’s Thesis, National Taiwan University, Taipei, Taiwan
Chen JP, Chang GY, Chen JK (2008) Electrospun collagen/chitosan nanofibrous membrane as wound dressing. Colloids Surf A 313–314:183–188
Chen CT, Huang Y, Zhu CL, Nie Y, Yang JZ, Sun DP (2014) Synthesis and characterization of hydroxypropyl cellulose from bacterial cellulose. Chin J Polym Sci 32:439–448
Çiplak Z, Yildiz N, Çalimli A (2015) Investigation of graphene/ag nanocomposites synthesis parameters for two different synthesis methods. Fuller Nanotub Carbon Nanostruct 23:361–370
Croisier F, Jérôme C (2013) Chitosan-based biomaterials for tissue engineering. Eur Polym J 49:780–792
Dhivya S, Padma VV, Santhini E (2015) Wound dressings—a review. BioMedicine 5:24–28
Ding YH, Ren HM, Chang FH, Zhang P, Jiang Y (2013) Intrinsic structure and friction properties of graphene and graphene oxide nanosheets studied by scanning probe microscopy. Bull Mater Sci 36:1073–1077
Goy RC, Morais STB, Assis OBG (2016) Evaluation of the antimicrobial activity of chitosan and its quaternized derivative on E. coli and S. aureus growth. Revista Brasileira de Farmacognosia 26:122–127
Hegab HM, ElMekawy A, Zou L, Mulcahy D, Saint CP, Ginic-Markovic M (2016) The controversial antibacterial activity of graphene-based materials. Carbon 105:362–376
Holbrook RD, Rykaczewski K, Staymates ME (2014) Dynamics of silver nanoparticle release from wound dressings revealed via in situ nanoscale imaging. J Mater Sci Mater Med 25:2481–2489
Ji H, Sun H, Qu X (2016) Antibacterial applications of graphene-based nanomaterials: recent achievements and challenges. Adv Drug Deliv Rev 105:176–189
Jin SG, Yousaf AM, Kim KS, Kim DW, Kim DS, Kim JK, Yong CS, Youn YS, Kim JO, Choi HG (2016) Influence of hydrophilic polymers on functional properties and wound healing efficacy of hydrocolloid based wound dressings. Int J Pharm 501:160–166
Kamoun EA, Kenawy E-RS, Chen X (2017) A review on polymeric hydrogel membranes for wound dressing applications: pva-based hydrogel dressings. J Adv Res 8:217–233
Knaul JZ, Hudson SM, Creber KAM (1999) Crosslinking of chitosan fibers with dialdehydes: proposal of a new reaction mechanism. J Polym Sci Part B: Polym Phys 37:1079–1094
Kubota N, Tatsumoto N, Sano T, Toya K (2000) A simple preparation of half n-acetylated chitosan highly soluble in water and aqueous organic solvents. Carbohyd Res 324:268–274
Kuo TY, Lin CM, Hung SC, Hsien TY, Wang DM, Hsieh HJ (2018) Incorporation and selective removal of space-forming nanofibers to enhance the permeability of cytocompatible nanofiber membranes for better cell growth. J Taiwan Inst Chem Eng 91:146–154
Liang D, Lu Z, Yang H, Gao J, Chen R (2016) Novel asymmetric wettable agnps/chitosan wound dressing: in vitro and in vivo evaluation. ACS Appl Mater Interfaces 8:3958–3968
Liu T, Liu Y, Liu M, Wang Y, He W, Shi G, Hu X, Zhan R, Luo G, Xing M, Wu J (2018) Synthesis of graphene oxide-quaternary ammonium nanocomposite with synergistic antibacterial activity to promote infected wound healing. Burns Trauma 6:16
Lu X, Feng X, Werber JR, Chu C, Zucker I, Kim JH, Osuji CO, Elimelech M (2017a) Enhanced antibacterial activity through the controlled alignment of graphene oxide nanosheets. Proc Natl Acad Sci 114:E9793–E9801
Lu Z, Gao J, He Q, Wu J, Liang D, Yang H, Chen R (2017b) Enhanced antibacterial and wound healing activities of microporous chitosan-ag/zno composite dressing. Carbohyd Polym 156:460–469
Mahmoudi N, Eslahi N, Mehdipour A, Mohammadi M, Akbari M, Samadikuchaksaraei A, Simchi A (2017) Temporary skin grafts based on hybrid graphene oxide-natural biopolymer nanofibers as effective wound healing substitutes: pre-clinical and pathological studies in animal models. J Mater Sci Mater Med 28:73
Mi FL, Shyu SS, Wu YB, Lee ST, Shyong JY, Huang RN (2001) Fabrication and characterization of a sponge-like asymmetric chitosan membrane as a wound dressing. Biomaterials 22:165–173
Mirjalili M, Zohoori S (2016) Review for application of electrospinning and electrospun nanofibers technology in textile industry. J Nanostruct Chem 6:207–213
Misra SK, Ramteke PW, Patil S, Pandey AC, Pandey H (2018) Tolnaftate–graphene composite-loaded nanoengineered electrospun scaffolds as efficient therapeutic dressing material for regimen of dermatomycosis. Appl Nanosc 8:1629–1640
Mohamed NA, Abd El-Ghany NAJC (2019) Synthesis, characterization and antimicrobial activity of novel aminosalicylhydrazide cross linked chitosan modified with multi-walled carbon nanotubes. Cellulose 26:1141–1156
Pang L, Dai C, Bi L, Guo Z, Fan J (2017) Biosafety and antibacterial ability of graphene and graphene oxide in vitro and in vivo. Nanoscale Res Lett 12:564
Park JU, Jeong SH, Song EH, Song J, Kim HE, Kim S (2018) Acceleration of the healing process of full-thickness wounds using hydrophilic chitosan–silica hybrid sponge in a porcine model. J Biomater Appl 32:1011–1023
Pawlicka A, Sabadini RC, Nunzi J-MJC (2018) Reversible light-induced solubility of disperse red 1 dye in a hydroxypropyl cellulose matrix. Cellulose 25:2083–2090
Pérez-Díaz M, Alvarado-Gomez E, Magaña-Aquino M, Sánchez-Sánchez R, Velasquillo C, Gonzalez C, Ganem-Rondero A, Martínez-Castañon G, Zavala-Alonso N, Martinez-Gutierrez F (2016) Anti-biofilm activity of chitosan gels formulated with silver nanoparticles and their cytotoxic effect on human fibroblasts. Mater Sci Eng C 60:317–323
Queen D, Gaylor JDS, Evans JH, Courtney JM, Reid WH (1987) The preclinical evaluation of the water vapour transmission rate through burn wound dressings. Biomaterials 8:367–371
Raafat D, Sahl HG (2009) Chitosan and its antimicrobial potential–a critical literature survey. Microb Biotechnol 2:186–201
Sahariah P, Másson M (2017) antimicrobial chitosan and chitosan derivatives: a review of the structure-activity relationship. Biomacromol 18:3846–3868
Saquing CD, Tang C, Monian B, Bonino CA, Manasco JL, Alsberg E, Khan SA (2013) Alginate–polyethylene oxide blend nanofibers and the role of the carrier polymer in electrospinning. Ind Eng Chem Res 52:8692–8704
Sarabahi S (2012) Recent advances in topical wound care. Indian Journal of Plastic Surgery 45:379–387
Schunck M, Neumann C, Proksch E (2005) Artificial barrier repair in wounds by semi-occlusive foils reduced wound contraction and enhanced cell migration and reepithelization in mouse skin. J Investig Dermatol 125:1063–1071
Selig HF, Lumenta DB, Giretzlehner M, Jeschke MG, Upton D, Kamolz LP (2012) The properties of an “ideal” burn wound dressing – What do we need in daily clinical practice? Results of a worldwide online survey among burn care specialists. Burns 38:960–966
Smiechowicz E, Niekraszewicz B, Kulpinski P, Dzitko K (2018) Antibacterial composite cellulose fibers modified with silver nanoparticles and nanosilica. Cellulose 25:3499–3517
Sophie ELB, Giuseppe T, Parikshit G, Chris C, Stephen JR (2017) Antibacterial properties of nonwoven wound dressings coated with manuka honey or methylglyoxal. Materials 10:954
Stockert JC, Blázquez-Castro A, Cañete M, Horobin RW, Villanueva Á (2012) MTT assay for cell viability: intracellular localization of the formazan product is in lipid droplets. Acta Histochem 114:785–796
Tu Y, Lv M, Xiu P, Huynh T, Zhang M, Castelli M, Liu Z, Huang Q, Fan C, Fang H, Zhou R (2013) Destructive extraction of phospholipids from escherichia coli membranes by graphene nanosheets. Nat Nanotechnol 8:594–601
Tuson HH, Weibel DB (2013) Bacteria-surface interactions. Soft Matter 9:4368–4380
Verlee A, Mincke S, Stevens CV (2017) Recent developments in antibacterial and antifungal chitosan and its derivatives. Carbohyd Polym 164:268–283
Wang S-D, Ma Q, Wang K, Chen H-W (2018) Improving antibacterial activity and biocompatibility of bioinspired electrospinning silk fibroin nanofibers modified by graphene oxide. ACS Omega 3:406–413
Wu X, Tan S, Xing Y, Pu Q, Wu M, Zhao JX (2017) Graphene oxide as an efficient antimicrobial nanomaterial for eradicating multi-drug resistant bacteria in vitro and in vivo. Colloids Surf B 157:1–9
Xu R, Xia H, He W, Li Z, Zhao J, Liu B, Wang Y, Lei Q, Kong Y, Bai Y, Yao Z, Yan R, Li H, Zhan R, Yang S, Luo G, Wu J (2016) Controlled water vapor transmission rate promotes wound-healing via wound re-epithelialization and contraction enhancement. Sci Rep 6:24596
Yuan Y, Hays MP, Hardwidge PR, Kim J (2017) Surface characteristics influencing bacterial adhesion to polymeric substrates. RSC Adv 7:14254–14261
Yüksel E, Karakeçili A (2014) Antibacterial activity on electrospun poly(lactide-co-glycolide) based membranes via magainin II grafting. Mater Sci Eng C 45:510–518
Zargar V, Asghari M, Dashti A (2015) A review on chitin and chitosan polymers: structure, chemistry, solubility, derivatives, and applications. ChemBioEng Rev 2:204–226
Zhang Q, Tu Q, Hickey ME, Xiao J, Gao B, Tian C, Heng P, Jiao Y, Peng T, Wang J (2018) Preparation and study of the antibacterial ability of graphene oxide-catechol hybrid polylactic acid nanofiber mats. Colloids Surf B 172:496–505
Zheng H, Ma R, Gao M, Tian X, Li Y-Q, Zeng L, Li R (2018) Antibacterial applications of graphene oxides: structure-activity relationships, molecular initiating events and biosafety. Sci Bull 63:133–142
Zhou C, Chu R, Wu R, Wu Q (2011) Electrospun polyethylene oxide/cellulose nanocrystal composite nanofibrous mats with homogeneous and heterogeneous microstructures. Biomacromol 12:2617–2625
Acknowledgments
This study was supported by the Ministry of Science and Technology, Taiwan (Grant Numbers: MOST 104-2221-E-002-174 and MOST 105-2221-E-002-202). Hydroxypropyl cellulose and graphene powder were kindly provided by Eternal Materials Co. (Kaohsiung, Taiwan).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Lin, CM., Chang, YC., Cheng, LC. et al. Preparation of graphene-embedded hydroxypropyl cellulose/chitosan/polyethylene oxide nanofiber membranes as wound dressings with enhanced antibacterial properties. Cellulose 27, 2651–2667 (2020). https://doi.org/10.1007/s10570-019-02940-w
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10570-019-02940-w