Biomaterials with the ability to self-heal and recover their structural integrity offer many advantages for applications in biomedicine. The past decade has witnessed the rapid emergence of a new class of self-healing biomaterials commonly termed injectable, or printable in the context of 3D printing. These self-healing injectable biomaterials, mostly hydrogels and other soft condensed matter based on reversible chemistry, are able to temporarily fluidize under shear stress and subsequently recover their original mechanical properties. Self-healing injectable hydrogels offer distinct advantages compared to traditional biomaterials. Most notably, they can be administered in a locally targeted and minimally invasive manner through a narrow syringe without the need for invasive surgery. Their moldability allows for a patient-specific intervention and shows great prospects for personalized medicine. Injected hydrogels can facilitate tissue regeneration in multiple ways owing to their viscoelastic and diffusive nature, ranging from simple mechanical support, spatiotemporally controlled delivery of cells or therapeutics, to local recruitment and modulation of host cells to promote tissue regeneration. Consequently, self-healing injectable hydrogels have been at the forefront of many cutting-edge tissue regeneration strategies. This study provides a critical review of the current state of self-healing injectable hydrogels for tissue regeneration. As key challenges toward further maturation of this exciting research field, we identify (i) the trade-off between the self-healing and injectability of hydrogels vs their physical stability, (ii) the lack of consensus on rheological characterization and quantitative benchmarks for self-healing injectable hydrogels, particularly regarding the capillary flow in syringes, and (iii) practical limitations regarding translation toward therapeutically effective formulations for regeneration of specific tissues. Hence, here we (i) review chemical and physical design strategies for self-healing injectable hydrogels, (ii) provide a practical guide for their rheological analysis, and (iii) showcase their applicability for regeneration of various tissues and 3D printing of complex tissues and organoids.

Self-Healing Injectable Hydrogels for Tissue Regeneration

Diabetic foot ulcers (DFU), one of the most serious complications of diabetes, are essentially chronic, nonhealing wounds caused by diabetic neuropathy, vascular disease, and bacterial infection. Given its pathogenesis, the DFU microenvironment is rather complicated and characterized by hyperglycemia, ischemia, hypoxia, hyperinflammation, and persistent infection. However, the current clinical therapies for DFU are dissatisfactory, which drives researchers to turn attention to advanced nanotechnology to address DFU therapeutic bottlenecks. In the last decade, a large number of multifunctional nanosystems based on the microenvironment of DFU have been developed with positive effects in DFU therapy, forming a novel concept of “DFU nanomedicine”. However, a systematic overview of DFU nanomedicine is still unavailable in the literature. This review summarizes the microenvironmental characteristics of DFU, presents the main progress of wound healing, and summaries the state‐of‐the‐art therapeutic strategies for DFU. Furthermore, the main challenges and future perspectives in this field are discussed and prospected, aiming to fuel and foster the development of DFU nanomedicines successfully.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202203308

Microenvironment‐Based Diabetic Foot Ulcer Nanomedicine

Intelligent management beyond therapeutic drug treating holds significant prospects in facilitating the recovery of intractable chronic wounds. Here, inspired by the flat and inclined structure of shark teeth, we present a shark tooth-inspired microneedle patch for intelligent wound management. By simply replicating negative molds fabricated by laser engraving and using origami, such a biomimetic microneedle patch can be fabricated easily and rapidly. The biomimetic structures endow the microneedle patch with stable adhesion during the long-term recovery process of chronic wounds. Porous ordered structures and a temperature-responsive hydrogel are utilized to construct a controllable drug release system on the microneedle patch. The microfluidic channel composed of microneedle arrays and porous ordered structures enables a microneedle patch with the capacity to analyze several inflammatory factors. In addition, MXene electronics was patterned on the microneedle patch in order to achieve sensitive motion monitoring. Also, it was demonstrated from in vivo diabetic rat experiments that recovery of full-thickness cutaneous wounds including stripe-shaped and circular wounds can be facilitated by employing the drug-loaded biomimetic microneedle patch.

Shark Tooth-Inspired Microneedle Dressing for Intelligent Wound Management.

Bacterial infection has become one of the leading causes of death worldwide, particularly in low-income countries. Despite the fact that antibiotics have provided successful management in bacterial infections, the long-term overconsumption and abuse of antibiotics has contributed to the emergence of multidrug resistant bacteria. To address this challenge, nanomaterials with intrinsic antibacterial properties or that serve as drug carriers have been substantially developed as an alternative to fight against bacterial infection. Systematically and deeply understanding the antibacterial mechanisms of nanomaterials is extremely important for designing new therapeutics. Recently, nanomaterials-mediated targeted bacteria depletion in either a passive or active manner is one of the most promising approaches for antibacterial treatment by increasing local concentration around bacterial cells to enhance inhibitory activity and reduce side effects. Passive targeting approach is widely explored by searching nanomaterial-based alternatives to antibiotics, while active targeting strategy relies on biomimetic or biomolecular surface feature that can selectively recognize targeted bacteria. In this review article, we summarize the recent developments in the field of targeted antibacterial therapy based on nanomaterials, which will promote more innovative thinking focusing on the treatment of multidrug-resistant bacteria. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/EXP.20210117

Recent advances in targeted antibacterial therapy basing on nanomaterials

Electrospinning has rapidly progressed over the past few decades as an easy and versatile way to fabricate fibers with diameters ranging from micrometers to tens of nanometers that present unique and intricate morphologies. This has led to the conception of new technologies and diverse methods that exploit the basic electrohydrodynamic phenomena of the electrospinning process, which has in turn led to the invention of novel apparatuses that have reshaped the field. Research on revamping conventional electrospinning has principally focused on achieving three key objectives: upscaling the process while retaining consistent morphological traits, developing 3D nanofibrous macrostructures, and formulating novel fiber configurations. This review introduces an extensive group of diverse electrospinning techniques and presents a comperative study based on the apparatus type and output. Then, each process's advantages and limitations are critically assessed to identify the bona fide practicability and relevance of each technological breakthrough. Finally, the outlook on future developments of advanced electrospinning technologies is outlined, with an emphasis on upscaling, translational research, sustainable manufacturing and prospective solutions to current shortcomings.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/admt.202201723

The History of Electrospinning: Past, Present, and Future Developments

Nanofibers reinforced injectable hydrogel with self-healing, antibacterial, and hemostatic properties for chronic wound healing.

Majority of human infectious diseases is related to bacterial biofilm formation, especially the wound infection and delayed healing. Herein, recognizing peptide-modified polysaccharide based injectable hydrogel has been synthesized for effective anti-biofilm and infected wound healing. Inspiration from similar compatibility principle, the peptide (Alanine-glutamate-lysine-alanine), which is a part of the peptidoglycan, is grafted into the quaternized carboxymethyl chitosan （HTCC）for the first time. Afterwards, the quaternary ammonium salt groups in the synthetic injectable hydrogel cross-linked by the peptide modified quaternized carboxymethyl chitosan (HTCC-P) and oxidized dextran (OD), which can penetrate the bacterial cell wall and membrane under the recognition of peptide. Furthermore, the synergistic effect of quaternary ammonium salt groups and the peptide significantly enhance the anti-biofilm property of the hydrogels. In addition, the injectable hydrogel (HTCC-P/OD) cross-linked by Schiff base exhibits an excellent self-healing property and can completely cover the irregular wound shape. The cytotoxicity and in vivo wound healing also confirm the biocompatibility and capacity to accelerate tissue reconstruction of the hydrogels. Therefore, the hydrogels are expected to become competitive multifunctional dressings in biomedical field, including chronic wound infection and other bacterial biofilm related tissue repair.

Peptidoglycan-inspired peptide-modified injectable hydrogels with enhanced elimination capability of bacterial biofilm for chronic wound healing

Conductive hydrogel dressings based on cascade reactions with photothermal effect for monitoring and treatment of diabetic wounds

Multifunctional hydrogel platform for biofilm scavenging and O2 generating with photothermal effect on diabetic chronic wound healing.

Fabrication of eco-friendly and efficient flame retardant modified cellulose with antibacterial property.

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