Abstract
Nanocelluloses and cellulose nanomaterials derived from natural resources are a group of ideal platform materials for advanced applications. However, their synthesis through sustainable and facile processes to achieve the required properties are still challenging. Here, we prepare the nanocellulose oxalate (n-COX) from cotton with outstanding physicochemical properties by defining the optimal oxalic acid pretreatment conditions. Thus-obtained n-COX with unique 1D nanofiber shape as a platform material is further processed to various high-performance multidimensional bio-nanomaterials through several simple yet effective strategies. First, 2D n-COX films prepared through a casting-drying method show comparable or even better transparency and tensile strength than those made from other types of nanocelluloses. Second, 3D n-COX hydrogels/aerogels fabricated by a molding-crosslinking approach demonstrate good shape stability, well-preserved nanoporous networks, and qualified mechanical properties. Third, n-COX-derived bioinks display improved printability and fidelity, resulting in better size-preserving and shape-control of the 3D-bioprinted scaffolds. We expect this work could offer new insights on engineering natural cellulose and using n-COX as a platform material for further advanced fabrication, and thus, open up application potentials of this new nanocellulose.
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The datasets used and/or analysed during the current study available from the corresponding author on reasonable request.
References
Abitbol T, Kloser E, Gray DG (2013) Estimation of the surface sulfur content of cellulose nanocrystals prepared by sulfuric acid hydrolysis. Cellulose 20:785–794
Abouzeid RE, Khiari R, Beneventi D, Dufresne A (2018) Biomimetic mineralization of three-dimensional printed alginate/TEMPO-oxidized cellulose nanofibril scaffolds for bone tissue engineering. Biomacromol 19:4442–4452
Ahankari S, Paliwal P, Subhedar A, Kargarzadeh H (2021) Recent developments in nanocellulose-based aerogels in thermal applications: a review. ACS Nano 15:3849–3874
Ávila HM, Schwarz S, Rotter N, Gatenholm P (2016) 3D bioprinting of human chondrocyte-laden nanocellulose hydrogels for patient-specific auricular cartilage regeneration. Bioprinting 1:22–35
Barbash VA, Yaschenko OV, Alushkin SV, Kondratyuk AS, Posudievsky OY, Koshechko VG (2016) The effect of mechanochemical treatment of the cellulose on characteristics of nanocellulose films. Nanoscale Res Lett 11:410. https://doi.org/10.1186/s11671-016-1632-1
Chen W et al (2014) Comparative study of aerogels obtained from differently prepared nanocellulose fibers. ChemSusChem 7:154–161. https://doi.org/10.1002/cssc.201300950
Chinga-Carrasco G et al (2019) Bagasse—a major agro-industrial residue as potential resource for nanocellulose inks for 3D printing of wound dressing devices. Addit Manuf 28:267–274
Curvello R, Garnier G (2020) Cationic cross-linked nanocellulose-based matrices for the growth and recovery of intestinal organoids. Biomacromol 22:701–709
De Oliveira PB, Godinho M, Zattera AJ (2018) Oils sorption on hydrophobic nanocellulose aerogel obtained from the wood furniture industry waste. Cellulose 25:3105–3119
Golmohammadi H, Morales-Narváez E, Naghdi T, Merkoçi A (2017) Nanocellulose in sensing and biosensing. Chem Mater 29:5426–5446
Hajiali F, Jin T, Yang G, Santos M, Lam E, Moores A (2022) Mechanochemical transformations of biomass into functional materials. ChemSusChem 15:e202102535. https://doi.org/10.1002/cssc.202102535
Henschen J, Li D, Ek M (2019) Preparation of cellulose nanomaterials via cellulose oxalates. Carbohydr Polym 213:208–216. https://doi.org/10.1016/j.carbpol.2019.02.056
Huang T, Li KD, Ek M (2021) Hydrophobization of cellulose oxalate using oleic acid in a catalyst-free esterification suitable for preparing reinforcement in polymeric composites. Carbohydr Polym 257:117615. https://doi.org/10.1016/j.carbpol.2021.117615
Ji Y, Wen Y, Wang Z, Zhang S, Guo M (2020) Eco-friendly fabrication of a cost-effective cellulose nanofiber-based aerogel for multifunctional applications in Cu (II) and organic pollutants removal. J Clean Prod 255:120276
Jia W, Liu Y (2019) Two characteristic cellulose nanocrystals (CNCs) obtained from oxalic acid and sulfuric acid processing. Cellulose 26:8351–8365. https://doi.org/10.1007/s10570-019-02690-9
Kopač T, Krajnc M, Ručigaj A (2021) A mathematical model for pH-responsive ionically crosslinked TEMPO nanocellulose hydrogel design in drug delivery systems. Int J Biol Macromol 168:695–707. https://doi.org/10.1016/j.ijbiomac.2020.11.126
Lei W, Jin D, Liu H, Tong Z, Zhang H (2020) An overview of bacterial cellulose in flexible electrochemical energy storage. ChemSusChem 13:3731–3753. https://doi.org/10.1002/cssc.202001019
Li Z, Liu J, Jiang K, Thundat T (2016) Carbonized nanocellulose sustainably boosts the performance of activated carbon in ionic liquid supercapacitors. Nano Energy 25:161–169
Li D, Henschen J, Ek M (2017) Esterification and hydrolysis of cellulose using oxalic acid dihydrate in a solvent-free reaction suitable for preparation of surface-functionalised cellulose nanocrystals with high yield. Green Chem 19:5564–5567. https://doi.org/10.1039/C7GC02489D
Liang L, Bhagia S, Li M, Huang C, Ragauskas AJ (2020) Cross-linked nanocellulosic materials and their applications. ChemSusChem 13:78–87. https://doi.org/10.1002/cssc.201901676
Liu Y, Sui Y, Liu C, Liu C, Wu M, Li B, Li Y (2018) A physically crosslinked polydopamine/nanocellulose hydrogel as potential versatile vehicles for drug delivery and wound healing. Carbohydr Polym 188:27–36
Lu C, Wang C, Yu J, Wang J, Chu F (2020) Two-step 3D-printing approach toward sustainable, repairable, fluorescent shape-memory thermosets derived from cellulose and rosin. ChemSusChem 13:893–902. https://doi.org/10.1002/cssc.201902191
Ma N, Cheung DY, Butcher JT (2022) Incorporating nanocrystalline cellulose into a multifunctional hydrogel for heart valve tissue engineering applications. J Biomed Mater Res A 110:76–91
Maturavongsadit P, Narayanan LK, Chansoria P, Shirwaiker R, Benhabbour SR (2021) Cell-laden nanocellulose/chitosan-based bioinks for 3D bioprinting and enhanced osteogenic cell differentiation. ACS Appl Bio Mater 4:2342–2353
Mi H, Li Y, Wang C, Yi S, Li X, Li J (2021) The interaction of starch-gums and their effect on gel properties and protein conformation of silver carp surimi. Food Hydrocoll 112:106290. https://doi.org/10.1016/j.foodhyd.2020.106290
Mo L et al (2021) Wood-inspired nanocellulose aerogel adsorbents with excellent selective pollutants capture, superfast adsorption, and easy regeneration. J Hazard Mater 415:125612
Montero Y, Souza AG, Oliveira ÉR, dos Rosa DS (2021) Nanocellulose functionalized with cinnamon essential oil: a potential application in active biodegradable packaging for strawberry. Sustain Mater Technol 29:e00289. https://doi.org/10.1016/j.susmat.2021.e00289
Nemoto J, Saito T, Isogai A (2015) Simple freeze-drying procedure for producing nanocellulose aerogel-containing, high-performance air filters. ACS Appl Mater Interfaces 7:19809–19815
Piras CC, Fernández-Prieto S, De Borggraeve WM (2017) Nanocellulosic materials as bioinks for 3D bioprinting. Biomater Sci 5:1988–1992
Ramakrishnan R, Kasoju N, Raju R, Geevarghese R, Gauthaman A, Bhatt A (2022) Exploring the potential of alginate-gelatin-diethylaminoethyl cellulose-fibrinogen based bioink for 3D bioprinting of skin tissue constructs. Carbohydr Polym Technol Appl 3:100184
Reising AB, Moon RJ, Youngblood JP (2012) Effect of particle alignment on mechanical properties of neat cellulose nanocrystal films. J Sci Technol For Prod Process 2:32–41
Saito T, Kimura S, Nishiyama Y, Isogai A (2007) Cellulose nanofibers prepared by TEMPO-mediated oxidation of native cellulose. Biomacromol 8:2485–2491. https://doi.org/10.1021/bm0703970
Shanmugam K, Doosthosseini H, Varanasi S, Garnier G, Batchelor W (2019) Nanocellulose films as air and water vapour barriers: a recyclable and biodegradable alternative to polyolefin packaging. Sustain Mater Technol 22:e00115. https://doi.org/10.1016/j.susmat.2019.e00115
Shi C et al (2021) Sustainable and superhydrophobic spent coffee ground-derived holocellulose nanofibers foam for continuous oil/water separation. Sustain Mater Technol 28:e00277. https://doi.org/10.1016/j.susmat.2021.e00277
Shojaeiarani J, Bajwa DS, Stark NM, Bergholz TM, Kraft AL (2020) Spin coating method improved the performance characteristics of films obtained from poly(lactic acid) and cellulose nanocrystals. Sustain Mater Technol 26:e00212. https://doi.org/10.1016/j.susmat.2020.e00212
Sun B, Zhang M, Hou Q, Liu R, Wu T, Si C (2016) Further characterization of cellulose nanocrystal (CNC) preparation from sulfuric acid hydrolysis of cotton fibers. Cellulose 23:439–450. https://doi.org/10.1007/s10570-015-0803-z
Tao P, Wu Z, Xing C, Zhang Q, Wei Z, Nie S (2019) Effect of enzymatic treatment on the thermal stability of cellulose nanofibrils. Cellulose 26:7717–7725
Vilarinho F, Sanches Silva A, Vaz MF, Farinha JP (2018) Nanocellulose in green food packaging. Crit Rev Food Sci Nutr 58:1526–1537
Vilela C, Silvestre AJD, Figueiredo FML, Freire CSR (2019) Nanocellulose-based materials as components of polymer electrolyte fuel cells. J Mater Chem A 7:20045–20074. https://doi.org/10.1039/C9TA07466J
Vollick B, Kuo P-Y, Thérien-Aubin H, Yan N, Kumacheva E (2017) Composite cholesteric nanocellulose films with enhanced mechanical properties. Chem Mater 29:789–795. https://doi.org/10.1021/acs.chemmater.6b04780
Wakabayashi M, Fujisawa S, Saito T, Isogai A (2020) Nanocellulose film properties tunable by controlling degree of fibrillation of TEMPO-oxidized cellulose. Front Chem 8:37. https://doi.org/10.3389/fchem.2020.00037
Wang R, Chen L, Zhu JY, Yang R (2017) Tailored and integrated production of carboxylated cellulose nanocrystals (CNC) with nanofibrils (CNF) through maleic acid hydrolysis. ChemNanoMat 3:328–335. https://doi.org/10.1002/cnma.201700015
Wang Q, Sun J, Yao Q, Ji C, Liu J, Zhu Q (2018) 3D printing with cellulose materials. Cellulose 25:4275–4301
Wei J et al (2019) Carboxymethyl cellulose nanofibrils with a treelike matrix: preparation and behavior of pickering emulsions stabilization. ACS Sustain Chem Eng 7:12887–12896. https://doi.org/10.1021/acssuschemeng.9b01822
Wu Y, Lin ZY, Wenger AC, Tam KC, Tang X (2018) 3D bioprinting of liver-mimetic construct with alginate/cellulose nanocrystal hybrid bioink. Bioprinting 9:1–6. https://doi.org/10.1016/j.bprint.2017.12.001
Xie H, Du H, Yang X, Si C (2018) Recent strategies in preparation of cellulose nanocrystals and cellulose nanofibrils derived from raw cellulose materials. Int J Polym Sci 2018:7923068. https://doi.org/10.1155/2018/7923068
Xie H et al (2019) Preparation of thermally stable and surface-functionalized cellulose nanocrystals via mixed H2SO4/Oxalic acid hydrolysis. Carbohydr Polym 223:115116. https://doi.org/10.1016/j.carbpol.2019.115116
Xing X, Li W, Zhang J, Wu H, Guan Y, Gao H (2021) TEMPO-oxidized cellulose hydrogel for efficient adsorption of Cu2+ and Pb2+ modified by polyethyleneimine. Cellulose 28:7953–7968. https://doi.org/10.1007/s10570-021-04052-w
Xu L, Xiong Y, Dang B, Wang C, Jin C, Sun Q, Zhang X (2017a) Utilizing cellulose sheets as structure promoter constructing different micro-nano titanate nanotubes networks for green water purification. Carbohydr Polym 175:756–764
Xu W et al (2017b) Mild oxalic-acid-catalyzed hydrolysis as a novel approach to prepare cellulose nanocrystals. ChemNanoMat 3:109–119. https://doi.org/10.1002/cnma.201600347
Xu Y, Yang S, Zhao P, Wu M, Song X, Ragauskas AJ (2021) Effect of endoglucanase and high-pressure homogenization post-treatments on mechanically grinded cellulose nanofibrils and their film performance. Carbohydr Polym 253:117253. https://doi.org/10.1016/j.carbpol.2020.117253
Zander NE, Dong H, Steele J, Grant JT (2014) Metal cation cross-linked nanocellulose hydrogels as tissue engineering substrates. ACS Appl Mater Interfaces 6:18502–18510
Zhao Y, Li J (2014) Excellent chemical and material cellulose from tunicates: diversity in cellulose production yield and chemical and morphological structures from different tunicate species. Cellulose 21:3427–3441. https://doi.org/10.1007/s10570-014-0348-6
Zhao Y, Zhang Y, Lindstrom ME, Li J (2015) Tunicate cellulose nanocrystals: preparation, neat films and nanocomposite films with glucomannans. Carbohydr Polym 117:286–296. https://doi.org/10.1016/j.carbpol.2014.09.020
Zhao Y, Moser C, Lindström ME, Henriksson G, Li J (2017) Cellulose nanofibers from softwood, hardwood, and tunicate: preparation–structure–film performance interrelation. ACS Appl Mater Interfaces 9:13508–13519. https://doi.org/10.1021/acsami.7b01738
Zhong Y, Seidi F, Li C, Wan Z, Jin Y, Song J, Xiao H (2021) Antimicrobial/biocompatible hydrogels dual-reinforced by cellulose as ultrastretchable and rapid self-healing wound dressing. Biomacromol 22:1654–1663
Zhou J, Hsieh Y-L (2020) Nanocellulose aerogel-based porous coaxial fibers for thermal insulation. Nano Energy 68:104305
Zhou F, Wu S, Rader C, Ma J, Chen S, Yuan X, Foster EJ (2020) Crosslinked ionic alginate and cellulose-based hydrogels for photoresponsive drug release systems. Fibers Polym 21:45–54
Acknowledgments
Yadong Zhao is grateful for the financial support from Zhejiang Provincial Natural Science Foundation for Distinguished Young Scholars of China (No. LR23C160001), Zhejiang Ocean University (11135091221) and Science and Technology Planning Project of Zhoushan of China (No. 2022C41001).
Funding
Yadong Zhao is grateful for the financial support from Zhejiang Provincial Natural Science Foundation for Distinguished Young Scholars of China (No. LR23C160001), Zhejiang Ocean University (11135091221) and Science and Technology Planning Project of Zhoushan of China (No. 2022C41001).
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All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by YZ, JL and RZ. The first draft of the manuscript was written by YZ and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
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Zhao, Y., Li, J., Yu, Q. et al. Fabrication of multidimensional bio-nanomaterials from nanocellulose oxalate. Cellulose 30, 2147–2163 (2023). https://doi.org/10.1007/s10570-022-05019-1
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DOI: https://doi.org/10.1007/s10570-022-05019-1