Scholarly Works, Macromolecules Innovation Institute (MII)
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Browsing Scholarly Works, Macromolecules Innovation Institute (MII) by Department "Materials Science and Engineering"
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- Bioactive Cellulose Nanocrystal-Poly(epsilon-Caprolactone) Nanocomposites for Bone Tissue Engineering ApplicationsHong, Jung Ki; Cooke, Shelley L.; Whittington, Abby R.; Roman, Maren (2021-02-25)3D-printed bone scaffolds hold great promise for the individualized treatment of critical-size bone defects. Among the resorbable polymers available for use as 3D-printable scaffold materials, poly(epsilon-caprolactone) (PCL) has many benefits. However, its relatively low stiffness and lack of bioactivity limit its use in load-bearing bone scaffolds. This study tests the hypothesis that surface-oxidized cellulose nanocrystals (SO-CNCs), decorated with carboxyl groups, can act as multi-functional scaffold additives that (1) improve the mechanical properties of PCL and (2) induce biomineral formation upon PCL resorption. To this end, an in vitro biomineralization study was performed to assess the ability of SO-CNCs to induce the formation of calcium phosphate minerals. In addition, PCL nanocomposites containing different amounts of SO-CNCs (1, 2, 3, 5, and 10 wt%) were prepared using melt compounding extrusion and characterized in terms of Young's modulus, ultimate tensile strength, crystallinity, thermal transitions, and water contact angle. Neither sulfuric acid-hydrolyzed CNCs (SH-CNCs) nor SO-CNCs were toxic to MC3T3 preosteoblasts during a 24 h exposure at concentrations ranging from 0.25 to 3.0 mg/mL. SO-CNCs were more effective at inducing mineral formation than SH-CNCs in simulated body fluid (1x). An SO-CNC content of 10 wt% in the PCL matrix caused a more than 2-fold increase in Young's modulus (stiffness) and a more than 60% increase in ultimate tensile strength. The matrix glass transition and melting temperatures were not affected by the SO-CNCs but the crystallization temperature increased by about 5.5 degrees C upon addition of 10 wt% SO-CNCs, the matrix crystallinity decreased from about 43 to about 40%, and the water contact angle decreased from 87 to 82.6 degrees. The abilities of SO-CNCs to induce calcium phosphate mineral formation and increase the Young's modulus of PCL render them attractive for applications as multi-functional nanoscale additives in PCL-based bone scaffolds.
- A critical review of the current knowledge regarding the biological impact of nanocelluloseEndes, Carola; Camarero-Espinosa, Sandra; Mueller, Silvana; Foster, Earl Johan; Petri-Fink, Alke; Rothen-Rutishauser, Barbara; Weder, Christoph; Clift, Martin James David (2016-12-01)Several forms of nanocellulose, notably cellulose nanocrystals and nanofibrillated cellulose, exhibit attractive property matrices and are potentially useful for a large number of industrial applications. These include the paper and cardboard industry, use as reinforcing filler in polymer composites, basis for low-density foams, additive in adhesives and paints, as well as a wide variety of food, hygiene, cosmetic, and medical products. Although the commercial exploitation of nanocellulose has already commenced, little is known as to the potential biological impact of nanocellulose, particularly in its raw form. This review provides a comprehensive and critical review of the current state of knowledge of nanocellulose in this format. Overall, the data seems to suggest that when investigated under realistic doses and exposure scenarios, nanocellulose has a limited associated toxic potential, albeit certain forms of nanocellulose can be associated with more hazardous biological behavior due to their specific physical characteristics.
- Elucidating the Potential Biological Impact of Cellulose NanocrystalsCamarero-Espinosa, Sandra; Endes, Carola; Mueller, Silvana; Petri-Fink, Alke; Rothen-Rutishauser, Barbara; Weder, Christoph; Clift, Martin James David; Foster, Earl Johan (MDPI, 2016-07-08)Cellulose nanocrystals exhibit an interesting combination of mechanical properties and physical characteristics, which make them potentially useful for a wide range of consumer applications. However, as the usage of these bio-based nanofibers increases, a greater understanding of human exposure addressing their potential health issues should be gained. The aim of this perspective is to highlight how knowledge obtained from studying the biological impact of other nanomaterials can provide a basis for future research strategies to deduce the possible human health risks posed by cellulose nanocrystals.
- Functionalized Cellulose Nanocrystal Nanocomposite Membranes with Controlled Interfacial Transport for Improved Reverse Osmosis PerformanceSmith, Ethan D.; Hendren, Keith D.; Haag, James; Foster, Earl Johan; Martin, Stephen M. (MDPI, 2019-01-20)Thin-film nanocomposite membranes (TFNs) are a recent class of materials that use nanoparticles to provide improvements over traditional thin-film composite (TFC) reverse osmosis membranes by addressing various design challenges, e.g., low flux for brackish water sources, biofouling, etc. In this study, TFNs were produced using as-received cellulose nanocrystals (CNCs) and 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanocrystals (TOCNs) as nanoparticle additives. Cellulose nanocrystals are broadly interesting due to their high aspect ratios, low cost, sustainability, and potential for surface modification. Two methods of membrane fabrication were used in order to study the effects of nanoparticle dispersion on membrane flux and salt rejection: a vacuum filtration method and a monomer dispersion method. In both cases, various quantities of CNCs and TOCNs were incorporated into a polyamide TFC membrane via in-situ interfacial polymerization. The flux and rejection performance of the resulting membranes was evaluated, and the membranes were characterized via attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), transmission electron microscopy (TEM), and atomic force microscopy (AFM). The vacuum filtration method resulted in inconsistent TFN formation with poor nanocrystal dispersion in the polymer. In contrast, the dispersion method resulted in more consistent TFN formation with improvements in both water flux and salt rejection observed. The best improvement was obtained via the monomer dispersion method at 0.5 wt% TOCN loading resulting in a 260% increase in water flux and an increase in salt rejection to 98.98 ± 0.41% compared to 97.53 ± 0.31% for the plain polyamide membrane. The increased flux is attributed to the formation of nanochannels at the interface between the high aspect ratio nanocrystals and the polyamide matrix. These nanochannels serve as rapid transport pathways through the membrane, and can be used to tune selectivity via control of particle/polymer interactions.
- Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion BioprintingFrost, Brody A.; Sutliff, Bradley P.; Thayer, Patrick; Bortner, Michael J.; Foster, Earl Johan (2019-10-18)Bioprinting has advanced drastically in the last decade, leading to many new biomedical applications for tissue engineering and regenerative medicine. However, there are still a myriad of challenges to overcome, with vast amounts of research going into bioprinter technology, biomaterials, cell sources, vascularization, innervation, maturation, and complex 4D functionalization. Currently, stereolithographic bioprinting is the primary technique for polymer resin bioinks. However, it lacks the ability to print multiple cell types and multiple materials, control directionality of materials, and place fillers, cells, and other biological components in specific locations among the scaffolds. This study sought to create bioinks from a typical polymer resin, poly(ethylene glycol) diacrylate (PEGDA), for use in extrusion bioprinting to fabricate gradient scaffolds for complex tissue engineering applications. Bioinks were created by adding cellulose nanocrystals (CNCs) into the PEGDA resin at ratios from 95/5 to 60/40 w/w PEGDA/CNCs, in order to reach the viscosities needed for extrusion printing. The bioinks were cast, as well as printed into single-material and multiple-material (gradient) scaffolds using a CELLINK BIOX printer, and crosslinked using lithium phenyl-2,4,6-trimethylbenzoylphosphinate as the photoinitiator. Thermal and mechanical characterizations were performed on the bioinks and scaffolds using thermogravimetric analysis, rheology, and dynamic mechanical analysis. The 95/5 w/w composition lacked the required viscosity to print, while the 60/40 w/w composition displayed extreme brittleness after crosslinking, making both CNC compositions non-ideal. Therefore, only the bioink compositions of 90/10, 80/20, and 70/30 w/w were used to produce gradient scaffolds. The gradient scaffolds were printed successfully and embodied unique mechanical properties, utilizing the benefits of each composition to increase mechanical properties of the scaffold as a whole. The bioinks and gradient scaffolds successfully demonstrated tunability of their mechanical properties by varying CNC content within the bioink composition and the compositions used in the gradient scaffolds. Although stereolithographic bioprinting currently dominates the printing of PEGDA resins, extrusion bioprinting will allow for controlled directionality, cell placement, and increased complexity of materials and cell types, improving the reliability and functionality of the scaffolds for tissue engineering applications.
- Isolation of Thermally Stable Cellulose Nanocrystals from Spent Coffee Grounds via Phosphoric Acid HydrolysisFrost, Brody A.; Foster, Earl Johan (2020-02-01)As the world's population exponentially grows, so does the need for the production of food, with cereal production growing annually from an estimated 1.0 billion to 2.5 billion tons within the last few decades. This rapid growth in food production results in an ever increasing amount of agricultural wastes, of which already occupies nearly 50% of the total landfill area. For example, is the billions of dry tons of cellulose-containing spent coffee grounds disposed in landfills annually. This paper seeks to provide a method for isolating cellulose nanocrystals (CNCs) from spent coffee grounds, in order to recycle and utilize the cellulosic waste material which would otherwise have no applications. CNCs have already been shown to have vast applications in the polymer engineering field, mainly utilized for their high strength to weight ratio for reinforcement of polymer-based nanocomposites. A successful method of purifying and hydrolyzing the spent coffee grounds in order to isolate usable CNCs was established. The CNCs were then characterized using current techniques to determine important chemical and physical properties. A few crucial properties determined were aspect ratio of 12 +/- 3, crystallinity of 74.2%, surface charge density of (48.4 +/- 6.2) mM/kg cellulose, and the ability to successfully reinforce a polymer based nanocomposite. These characteristics compare well to other literature data and common commercial sources of CNCs.
- Materials for the Spine: Anatomy, Problems, and SolutionsFrost, Brody A.; Camarero-Espinosa, Sandra; Foster, Earl Johan (MDPI, 2019-01-14)Disc degeneration affects 12% to 35% of a given population, based on genetics, age, gender, and other environmental factors, and usually occurs in the lumbar spine due to heavier loads and more strenuous motions. Degeneration of the extracellular matrix (ECM) within reduces mechanical integrity, shock absorption, and swelling capabilities of the intervertebral disc. When severe enough, the disc can bulge and eventually herniate, leading to pressure build up on the spinal cord. This can cause immense lower back pain in individuals, leading to total medical costs exceeding $100 billion. Current treatment options include both invasive and noninvasive methods, with spinal fusion surgery and total disc replacement (TDR) being the most common invasive procedures. Although these treatments cause pain relief for the majority of patients, multiple challenges arise for each. Therefore, newer tissue engineering methods are being researched to solve the ever-growing problem. This review spans the anatomy of the spine, with an emphasis on the functions and biological aspects of the intervertebral discs, as well as the problems, associated solutions, and future research in the field.