We developed a simple and one-step method to prepare biocompatible composites from cellulose (CEL) and chitosan (CS). [BMIm+Cl−], an ionic liquid (IL), was used as a green solvent to dissolve and prepare the [CEL+CS] composites. Since majority (>88%) of IL used was recovered for reuse by distilling the aqueous washings of [CEL+CS], the method is recyclable. XRD, FTIR, NIR, 13C CP-MAS-NMR and SEM were used to monitor the dissolution and to characterize the composites. The composite was found to have combined advantages of their components: superior mechanical strength (from CEL) and excellent adsorption capability for microcystin-LR, a deadly toxin produced by cyanobacteria (from CS). Specifically, the mechanical strength of the composites increased with CEL loading; e.g., up to 5X increase in tensile strength was achieved by adding 80% of CEL into CS. Kinetic results of adsorption confirm that unique properties of CS remain intact in the composite, i.e., it is not only a very good adsorbent for microcystin but also is better than all other available adsorbents. For example, it can adsorb 4X times more microcystin than the best reported adsorbent. Importantly, the microcystin adsorbed can be quantitatively desorbed to enable the composite to be reused with similar adsorption efficiency.
We have successfully developed a simple and totally recyclable method to synthesize novel, biocompatible and biodegradable composite materials from cellulose (CEL) and chitosan (CS). In this method, [BMIm+Cl−], an ionic liquid (IL), was used as a green solvent to dissolve and synthesize the [CEL+CS] composites. Since the IL can be removed from the composites by washing them with water, and recovered by distilling the washed solution, the method is totally recyclable. Spectroscopic and imaging techniques including XRD, FTIR, NIR and SEM were used to monitor the dissolution, to characterize and to confirm that CEL and CS were successfully regenerated. More importantly, we have successfully demonstrated that [CEL+CS] composite is particularly suited for many applications including antimicrobial property. This is because the composites have combined advantages of their components, namely superior chemical and mechanical stability (from CEL) and bactericide (from CS). Results of tensile strength measurements clearly indicate that adding CEL into CS substantially increase its tensile strength. Up to 5X increase in tensile strength can be achieved by adding 80% of CEL into CS. Results of in vitro antibacterial assays confirm that CS retains its antibacterial property in the composite. More importantly, the composites reported here can inhibit growth of wider range of bacteria than other CS-based materials prepared by conventional methods; i.e., over 24 hr period, the composites substantially inhibited growth of bacteria such as MRSA, VRE, S. aureus, E. coli. These are bacteria which are often found to have the highest morbidity and mortality associated with wound infections.
Chitosan (CS), a polysaccharide derived from chitin, the second most abundant polysaccharide, is widely used in the medical world because of its natural and nontoxic properties and its innate ability for antibacterial and hemostasis effects. In this study, the novel composites containing CS and cellulose (CEL) (i.e., [CEL + CS]), which we have previously synthesized using a green and totally recyclable method, were investigated for their antimicrobial activity, absorption of anticoagulated whole blood, anti-inflammatory activity through the reduction of tumor necrosis factor-α (TNF-α) and interleukin-6 (IL-6), and the biocompatibility with human fibroblasts. The [CEL + CS] composites were found to inhibit the growth of both Gram positive and negative microorganisms. For examples, the regenerated 100% lyophilized chitosan material was found to reduce growth of Escherichia coli (ATCC 8739 and vancomycin resistant Enterococcus faecalis (ATCC 51299) by 78, 36, and 64%, respectively. The composites are nontoxic to fibroblasts; that is, fibroblasts, which are critical to the formation of connective tissue matrix were found to grow and proliferate in the presence of the composites. They effectively absorb blood, and at the same rate and volume as commercially available wound dressings. The composites, in both air-dried and lyophilized forms, significantly inhibit the production of TNF-α and IL-6 by stimulated macrophages. These results clearly indicate that the biodegradable, biocompatible and nontoxic [CEL + CS] composites, particularly those dried by lyophilizing, can be effectively used as a material in wound dressings.
We have successfully developed a simple and one step method to prepare high performance supramolecular polysaccharide composites from cellulose (CEL), chitosan (CS) and (2,3,6-tri-O-acetyl)-α-, β- and γ-cyclodextrin (α-, β- and γ-TCD). In this method, [BMIm+Cl−], an ionic liquid (IL), was used as a solvent to dissolve and prepare the composites. Since majority (>88%) of the IL used was recovered for reuse, the method is recyclable. XRD, FT-IR, NIR and SEM were used to monitor the dissolution process and to confirm that the polysaccharides were regenerated without any chemical modifications. It was found that unique properties of each component including superior mechanical properties (from CEL), excellent adsorbent for pollutants and toxins (from CS) and size/structure selectivity through inclusion complex formation (from TCDs) remain intact in the composites. Specifically, results from kinetics and adsorption isotherms show that while CS-based composites can effectively adsorb the endocrine disruptors (polychlrophenols, bisphenol-A), its adsorption is independent on the size and structure of the analytes. Conversely, the adsorption by γ-TCD-based composites exhibits strong dependency on size and structure of the analytes. For example, while all three TCD-based composites (i.e., α-, β- and γ-TCD) can effectively adsorb 2-, 3- and 4-chlorophenol, only γ-TCD-based composite can adsorb analytes with bulky groups including 3,4-dichloro- and 2,4,5-trichlorophenol. Furthermore, equilibrium sorption capacities for the analytes with bulky groups by γ-TCD-based composite are much higher than those by CS-based composites. Together, these results indicate that γ-TCD-based composite with its relatively larger cavity size can readily form inclusion complexes with analytes with bulky groups, and through inclusion complex formation, it can strongly adsorb much more analytes and with size/structure selectivity compared to CS-based composites which can adsorb the analyte only by surface adsorption.
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