Advanced Bacterial Cellulose Ionic Conductors with Gigantic Thermopower for Low-Grade Heat Harvesting.

Ionic conductors such as polymer electrolytes and ionic liquids have high thermoelectric voltages several orders of magnitude higher than electronic thermoelectric materials, while their conductivity is much lower than the latter. This work reports a novel approach to achieve high-performance ionic conductors using calcium ion (Ca2+) coordinated bacterial cellulose (CaBC) through molecular channel engineering. Through the coordination of Ca2+ with cellulose molecular chain, the distance between the cellulose molecular chains is widened, so that ions can transport along the cellulose molecular chain. Therefore, we reported ionic thermoelectric (i-TE) material based on CaBC/NaCl with a relatively high ionic Seebeck coefficient of -27.2 mV K-1 and high ionic conductivity of 204.2 mS cm-1. This ionic hydrogel is promising in the design of high-thermopower i-TE materials for low-grade heat energy harvesting.

Covalently grafting polycation to bacterial cellulose for antibacterial and anti-cell adhesive wound dressings.

Hydrogel-based wound dressings are becoming increasingly important for wound healing. Bacterial cellulose (BC) has been commonly used as wound dressings due to its good in vitro and in vivo biocompatibility. However, pure BC does not possess antibacterial properties. In this regard, polycation gel was grafted onto the BC using a surface-initiated activator regenerated by electron transfer atom transfer radical polymerization (SI-ARGET ATRP) with subsequent quaternization for antibacterial wound dressing. Dimethylethyl methacrylate (DMAEMA) was successfully polymerized on the BC surface which was confirmed by Fourier transform infrared spectroscopy and elemental analysis. The morphology structure, specific surface area, pore size, and mechanical properties were also characterized. The quaternized PDMAEMA grafted on the BC endowed it with excellent antibacterial activity against E. coli (Gram-negative) and S. aureus (Gram-positive) with a killing rate of 89.2 % and 93.4 %, respectively. The number of cells was significantly reduced on QPD/BC hydrogel, demonstrating its good anti-adhesion ability. In vitro cellular evaluation revealed that the antibacterial wound dressing exhibited good biocompatibility. Overall, this study provides a feasible method to develop antibacterial and anti-cell adhesive hydrogel, which has a promising potential for wound healing.

Bacterial cellulose-based hydrogel with antibacterial activity and vascularization for wound healing.

Skin wounds need an appropriate wound dressing to help prevent bacterial infection and accelerate wound closure. Bacterial cellulose (BC) with a three-dimensional (3D) network structure is an important commercial dressing. However, how to effectively load antibacterial agents and balance the antibacterial activity is a lingering issue. Herein, this study aims to develop a functional BC hydrogel containing silver-loaded zeolitic imidazolate framework-8 (ZIF-8) antibacterial agent. The tensile strength of the prepared biopolymer dressing is >1 MPa, the swelling property is over 3000 %, the temperature can reach 50 °C in 5 min with near-infrared (NIR) and the release of Ag+ and Zn2+ is stable. In vitro investigation shows that the hydrogel displays enhanced antibacterial activity, and the bacteria survival ratios are only 0.85 % and 0.39 % against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). In vitro cell experiments present that BC/polydopamine/ZIF-8/Ag (BC/PDA/ZIF-8/Ag) shows satisfactory biocompatibility and promising angiogenic ability. In vivo study, the full-thickness skin defect on rats demonstrates remarkably wound healing ability and accelerated skin re-epithelialization. This work presents a competitive functional dressing with effective antibacterial properties and accelerative angiogenesis activities for wound repair.

Self-Stretchable Fiber Liquid Sensors Made with Bacterial Cellulose/Carbon Nanotubes for Smart Diapers.

Liquid sensors for detecting water and body fluids are crucial in daily water usage and health monitoring, but it is challenging to combine sensing performance with high tensile deformation and multifunctional applications. Here, a substrate-free, self-stretchable bacterial cellulose (BC)/carbon nanotube (CNT) helical fiber liquid sensor was prepared by the solution spinning and coiling process using BC as the water-sensitive matrix and CNTs as the active sensing materials. The BC/CNT (BCT) fiber sensor has a high stretch ratio of more than 1000% and a rapid response for a current change rate of 104% within 1 s, which is almost unaffected under washing and various stretching or knotting deformations. By combination of the BCT fiber, we can design smart diapers or water level detectors, which rapidly monitor the status of smart diapers or water level, and the monitoring result can be transferred on time through an alarm device or smartphone. In short, the scalable and continuous preparation of the self-stretchable BCT helical fiber will provide a capacious platform for the development of a wearable sensor applied in daily life (such as smart diapers, water level detection, etc.).

Anti-Fouling, Adhesive Polyzwitterionic Hydrogel Electrodes Toughened Using a Tannic Acid Nanoflower.

Conductive polyzwitterionic hydrogels with good adhesion properties show potential prospect in implantable electrodes and electronic devices. Adhesive property of polyzwitterionic hydrogels in humid environments can be improved by the introduction of catechol groups. However, common catechol modifiers can usually quench free radicals, resulting in a contradiction between long-term tissue adhesion and hydrogel toughness. By adding tannic acid (TA) to the dispersion of clay nanosheets and nanofibers, we designed TA-coated nanoflowers and nanofibers as the reinforcing phase to prepare polyzwitterionic hydrogels with adhesion properties. The hydrogel combines the mussel-like and zwitterionic co-adhesive mechanism to maintain long-term adhesion in underwater environments. In particular, the noncovalent cross-linking provided by the nanoflower structure effectively compensates for the defects caused by free-radical quenching so that the hydrogel obtained a high stretchability of over 2900% and a toughness of 1.16 J/m3. The hydrogel also has excellent anti-biofouling property and shows resistance to bacteria and cells. In addition, the hydrogel possesses a low modulus (<10 kPa) and ionic conductivity (0.25 S/m), making it an ideal material for the preparation of implantable electrodes.

Bacterial cellulose reinforced chitosan-based hydrogel with highly efficient self-healing and enhanced antibacterial activity for wound healing.

Biocompatible hydrogels with versatile functions are highly desired for demanding the complicated tissue issues, including irregular site and motional wound. Herein, a bio-based hydrogel with multifunctional properties is designed based on quaternized chitosan and dialdehyde bacterial cellulose. As a functional wound dressing, the hydrogel shows rapid self-healing performance and injectable behaviors due to dynamic Schiff-base interactions and presents superior antibacterial activity against E. coli (gram-negative) and S. aureus (gram-positive). The constructed 3D hydrogel also exhibits proper compressive property, desired water retention capacity. To be mentioned, the hydrogel could mimic the structure of natural extracellular matrix (ECM) in the presence of bacterial cellulose nanofibers. Thus, the biopolymer-based hydrogel shows good biocompatibility in terms of cell proliferation and cell spreading. The prepared chitosan-based hydrogel with self-healing, antibacterial, and low cost will become a promising biomaterial for wound healing.

Anisotropic bacterial cellulose hydrogels with tunable high mechanical performances, non-swelling and bionic nanofluidic ion transmission behavior.

Water-rich hydrogels with tissue-like softness, especially ion conductive hydrogels with ion signal transfer systems similar to biological areas, are promising soft electrode materials, while too poor or unstable mechanical properties that come from uncontrollable swelling and biocompatibility issues caused by introducing high concentration ions are serious obstacles in practical applications. Herein, a simple method for fabricating strong, stable, ion-conductive, anisotropic bacterial cellulose hydrogels (ABCHs) is first reported. Relying on nanofibers with high aspect ratio in bacterial cellulose (BC), a tailor-made nanofiber-network-reinforced structure is constructed by controlled dissolution, followed by aligning them well via a simple fossilizing process under stretching. Therefore, tunable high mechanical performances can be achieved and the maximum tensile strength can reach 14.3 MPa with 70% water content. It is worth noting that ABCHs will not swell in water for 30 days and maintain 93% tensile strength. Most importantly, the unique nanofluid behaviors from nanochannels in nanofibers allow effective ion transport in ABCHs relying only on low concentrations of ions in body fluids (<300 mM), avoiding sacrificing biocompatibility to achieve useful conductivity. This facile strategy might be very scalable in fabricating high-strength, non-swelling, bio-ion conductive cellulose hydrogels for application in next-generation bio-interfacing and flexible implantable devices.

A 3D-printable TEMPO-oxidized bacterial cellulose/alginate hydrogel with enhanced stability via nanoclay incorporation.

Three-dimensional (3D) printing offers a novel approach to manufacture repeatable personalized structures for mass customization in medical fields. Considering the resemblance of materials in composition and microstructure to biological tissues, polysaccharide-based hydrogel is a promising printing material. However, its long-term stability of structure has always been a problem. In this work, we showed a green nanocomposite printing ink based on 2,2,6,6-tetramethylpiperidinyl-1-oxyl (TEMPO)-oxidized bacterial cellulose (TOBC), sodium alginate (SA) and laponite nanoclay (Xls). The TOBC/SA/Xls hydrogel prepared by the 3D printing ink not only exhibited structural stability, but also performed a long-term release behavior of protein which could be attractive in medical application of drug release, biomedical devices and tissue engineering.

Urethra-inspired biomimetic scaffold: A therapeutic strategy to promote angiogenesis for urethral regeneration in a rabbit model.

Limited angiogenesis and epithelialization make urethral regeneration using conventional tissue-engineered grafts a great challenge. Consequently, inspired from the native urethra, bacterial cellulose (BC) and bladder acellular matrix (BAM) were combined to design a three dimensional (3D) biomimetic scaffold. The developed BC/BAM scaffold was engineered for accelerating urethral regeneration by enhancing angiogenesis and epithelialization. The BC/BAM scaffold reveals the closest mimic of native urethra in terms of the 3D porous nanofibrous structure and component including collagen, glycosaminoglycans, and intrinsic vascular endothelial growth factor (VEGF). In vitro studies showed that the bioinspired BC/BAM scaffold promoted in vitro angiogenesis by facilitating human umbilical vein endothelial cells (HUVECs) growth, expression of endothelial function related proteins and capillary-like tube formation. Effect of the BC/BAM scaffold on angiogenesis and epithelialization was studied by its implantation in a rabbit urethral defect model for 1 and 3 months. Results demonstrated that the improved blood vessels formation in the urethra-inspired BC/BAM scaffold significantly promoted epithelialization and accelerated urethral regeneration. The urethra-inspired BC/BAM scaffold provides us a new design approach to construct grafts for urethral regeneration. STATEMENT OF SIGNIFICANCE: Findings in urethral regeneration demonstrate that an ideal tissue-engineered urethra should have adequate angiogenesis to support epithelialization for urethral regeneration in vivo. In this study, inspired from the native urethra, a bioinspired bacterial cellulose/bladder acellular matrix (BC/BAM) scaffold was developed to promote angiogenesis and epithelialization. The designed scaffold showed the closest physical structure and component to natural urethra, which is beneficial to angiogenesis and regeneration of urethral epithelium. This is the first time to utilize BC and dissolved BAM to develop biomimetic scaffold in urethral tissue engineering. Our biomimetic strategy on urethra graft design provided enhanced angiogenesis and epithelialization to achieve an accelerated and successful rabbit urethral repair. We believe that our urethra-inspired biomimetic scaffold would provide new insights into the design of urethral tissue engineering grafts.

A strategy of tailoring polymorphs and nanostructures to construct self-reinforced nonswelling high-strength bacterial cellulose hydrogels.

A serious decline in mechanical properties of polysaccharide hydrogels caused by swelling has always been a difficult problem which greatly limited their application especially in the medical field. Herein, nonswelling high-strength natural hydrogels based on self-reinforced double-crosslinked bacterial cellulose (SDBC) were prepared. Inspired by the concept of homogeneous composite materials, by regulating the ratio of LiOH/urea alkaline solvent, the aggregation structure and nanostructure of SDBC hydrogels can be controlled, thereby a unique nanofiber-network-self-reinforced (FNSR) structure was constructed and a new self-reinforcing mechanism is proposed. The prepared SDBC hydrogels have excellent mechanical properties at a high water content (>91%) for the combination of double-crosslinking and a unique FNSR structure, which can effectively prevent crack propagation and dissipate a large amount of energy. In particular, the compressive strength can reach 3.17 MPa which is 56 times that of native bacterial cellulose (BC). It is worth mentioning that no swelling occurs for the hydrogel, and the mechanical strength still remains in excess of 90% for 15 days in water, which is favorable for promising application in underwater equipment, implantable ionic devices, and tissue engineering scaffolds. This study also opens up a new horizon for the preparation of self-reinforced hydrogels.

Use of heparinized bacterial cellulose based scaffold for improving angiogenesis in tissue regeneration.

Vascularization is a prerequisite to achieve tissue regeneration especially for long-term survival of a scaffold. During the regeneration process, the delivery of angiogenic factors is very important for developing a vascular network. In this paper, vascular endothelial growth factor (VEGF)-loaded 3D porous bacterial cellulose/gelatin (B/G) scaffolds modified with heparin were firstly prepared. The pro-angiogenic effects of scaffolds towards proliferation and migration of endothelial cells (PIECs) were evaluated as well as in vivo implantation. Results showed that the B/G scaffold modified with heparin could provide a prolonged release of VEGF for two weeks. In vitro cellular assays showed that proliferation and migration were promoted in the presence of VEGF. Subcutaneous implantation demonstrated that angiogenesis was significantly improved for the heparinized scaffolds loaded with VEGF (V-B/G/H), compared to B/G scaffold. The resulting scaffold with sustained delivery of VEGF could be potential and effective tissue engineered candidates in tissue regeneration for future clinical applications.

Macrofibers with High Mechanical Performance Based on Aligned Bacterial Cellulose Nanofibers.

Bacterial cellulose (BC) nanofibers represent an emerging class of highly crystalline bionanofibers with high intrinsic mechanical properties. The remarkable nanofibers with oriented structure and strong interfibrillar interactions can realize high-performance materials. In this study, we demonstrated that macrofibers based on aligned BC nanofibers could be prepared by wet spinning and drawing procedures. The relationship between process conditions, structure, and mechanical properties of macrofibers were investigated. The obtained macrofibers exhibited Young's modulus of 16.4 GPa and tensile strength of 248.6 MPa under the optimum process conditions, in which nanofibers displayed a high degree of alignment. Furthermore, we enhanced the interfacial interactions between nanofibers and obtained better mechanical performance by multivalent ion cross-linking. After exchanging the monovalent Na+ by Fe3+, the dried macrofiber reached Young's modulus of 22.9 GPa and tensile strength of 357.5 MPa. Particularly, the resulting macrofibers still maintained good mechanical properties with Young's modulus of 15.9 GPa and tensile strength of 262.2 MPa in the wet condition. This research provided a good method to fabricate macrofibers from BC nanofibers with good properties by continuous wet-spinning process. These macrofibers can be easily functionalized and have promising potential applications in smart textiles, biosensor, and structural reinforcement.