Hydrogels for biomedical applications.

Polydopamine is one of the simplest and most versatile approaches to functionalizing material surfaces, having been inspired by the adhesive nature of catechols and amines in mussel adhesive proteins. Since its first report in 2007, a decade of studies on polydopamine molecular structure, deposition conditions, and physicochemical properties have ensued. During this time, potential uses of polydopamine coatings have expanded in many unforeseen directions, seemingly only limited by the creativity of researchers seeking simple solutions to manipulating surface chemistry. In this review, we describe the current state of the art in polydopamine coating methods, describe efforts underway to uncover and tailor the complex structure and chemical properties of polydopamine, and identify emerging trends and needs in polydopamine research, including the use of dopamine analogs, nitrogen-free polyphenolic precursors, and improvement of coating mechanical properties.

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Polydopamine Surface Chemistry: A Decade of Discovery.

The use of bone grafts is the standard to treat skeletal fractures, or to replace and regenerate lost bone, as demonstrated by the large number of bone graft procedures performed worldwide. The most common of these is the autograft, however, its use can lead to complications such as pain, infection, scarring, blood loss, and donor-site morbidity. The alternative is allografts, but they lack the osteoactive capacity of autografts and carry the risk of carrying infectious agents or immune rejection. Other approaches, such as the bone graft substitutes, have focused on improving the efficacy of bone grafts or other scaffolds by incorporating bone progenitor cells and growth factors to stimulate cells. An ideal bone graft or scaffold should be made of biomaterials that imitate the structure and properties of natural bone ECM, include osteoprogenitor cells and provide all the necessary environmental cues found in natural bone. However, creating living tissue constructs that are structurally, functionally and mechanically comparable to the natural bone has been a challenge so far. This focus of this review is on the evolution of these scaffolds as bone graft substitutes in the process of recreating the bone tissue microenvironment, including biochemical and biophysical cues.

Scaffold Design for Bone Regeneration

Hydrogels, due to their excellent biochemical and mechnical property, have shown attractive advantages in the field of wound dressings. However, a comprehensive review of the functional hydrogel as a wound dressing is still lacking. This work first summarizes the skin wound healing process and relates evaluation parameters and then reviews the advanced functions of hydrogel dressings such as antimicrobial property, adhesion and hemostasis, anti-inflammatory and anti-oxidation, substance delivery, self-healing, stimulus response, conductivity, and the recently emerged wound monitoring feature, and the strategies adopted to achieve these functions are all classified and discussed. Furthermore, applications of hydrogel wound dressing for the treatment of different types of wounds such as incisional wound and the excisional wound are summarized. Chronic wounds are also mentioned, and the focus of attention on infected wounds, burn wounds, and diabetic wounds is discussed. Finally, the future directions of hydrogel wound dressings for wound healing are further proposed.

Functional Hydrogels as Wound Dressing to Enhance Wound Healing.

In the last half-century, the development of biodegradable polymeric materials for biomedical applications has advanced significantly. Biodegradable polymeric materials are favored in the development of therapeutic devices, including temporary implants and three-dimensional scaffolds for tissue engineering. Further advancements have occurred in the utilization of biodegradable polymeric materials for pharmacological applications such as delivery vehicles for controlled/sustained drug release. These applications require particular physicochemical, biological, and degradation properties of the materials to deliver effective therapy. As a result, a wide range of natural or synthetic polymers able to undergo hydrolytic or enzymatic degradation is being studied for biomedical applications. This review outlines the current development of biodegradable natural and synthetic polymeric materials for various biomedical applications, including tissue engineering, temporary implants, wound healing, and drug delivery.

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Current development of biodegradable polymeric materials for biomedical applications

The accelerating and thorough treatment of chronic wounds still represents a major unmet medical need owing to the complex symptoms resulting from metabolic disorder of the wound microenvironment. Although numerous strategies and bioactive hydrogels are developed, an effective and widely used method of chronic wound treatment remains a bottleneck. With the aim to accelerate chronic wound healing, many hydrogel dressings with antioxidant functions have emerged and are proven to accelerate wound healing, especially for chronic wound repair. The new strategy in chronic wound treatment brought by antioxidant hydrogels is of great significance to human health. Here, the application of antioxidant hydrogels in the repair of chronic wounds is discussed systematically, aiming to provide an important theoretical reference for the further breakthrough of chronic wound healing.

Advances and Impact of Antioxidant Hydrogel in Chronic Wound Healing.

Polydopamine (PDA) has been increasingly exploited as an advanced functional material, and its emergent light absorption property plays a crucial role in determining various utilizations. However, the rational design and efficient regulation of PDA absorption property remain a challenge due to the complex structure within PDA. In this work, we propose a facile method to regulate the light absorption behaviors of PDA by constructing donor-acceptor pairs within the microstructures through the chemical connections between indoledihydroxy/indolequinone and their oligomers with 2,2,6,6-tetramethylpiperidine-1-oxyl moiety. The detailed structural and spectral analysis, as well as the density functional theory simulation, further confirms the existence of donor-acceptor molecular pair structures, which could decrease the energy bandgap and increase the electron delocalization for enhancing light absorption across a broad spectrum. These rationally designed PDA nanoparticles with tunable absorption properties also show improved total photothermal effect and demonstrate excellent performances in solar desalination.

Regulating the absorption spectrum of polydopamine

Effective bone regeneration remains a challenge for bone-tissue engineering. In this study, we propose a new strategy to accelerate bone regeneration via a sustained supply of phosphorus without providing foreign calcium. Herein, a black phosphorus nanosheet (BPN)-based hydrogel platform was developed, and the BPNs were used to stably and mildly provide phosphorus. The hydrogel was fabricated by photo-crosslinking of gelatin methacrylamide, BPNs, and cationic arginine-based unsaturated poly(ester amide)s. This platform combines the following advantages: the hydrogel scaffold would keep BPNs inside, and the encapsulated BPNs can degrade into phosphorus ions and capture calcium ions to accelerate biomineralization in a bone defect. The introduction of BPNs helped to enhance the mechanical performance of hydrogels, photoresponsively release phosphate, and accelerate mineralization in vitro. Moreover, BPN-containing hydrogels improved osteogenic differentiation of human dental pulp stem cells via the bone morphogenic protein-runt-related transcription factor 2 pathway. In vivo results from a rabbit model of bone defects revealed that the BPNs helped to accelerate bone regeneration. All these results strongly suggest that the strategy of a sustained supply of calcium-free phosphorus and this BPN-containing hydrogel platform hold promise for effective bone regeneration.

Black Phosphorus Hydrogel Scaffolds Enhance Bone Regeneration via a Sustained Supply of Calcium-Free Phosphorus.

Recently, the development of polydopamine (PDA) has demonstrated numerous excellent performances in free radical scavenging, UV shielding, photothermal conversion, and biocompatibility. These unique properties enable PDA to be widely used as efficient antibacterial materials for various applications. Accordingly, PDA antibacterial materials mainly include free-standing PDA materials and PDA-based composite materials. In this review, an overview of PDA antibacterial materials is provided to summarize these two types of antibacterial materials in detail, including the fabrication strategies and antibacterial mechanisms. The future development and challenges of PDA in this field are also presented. It is hoped that this review will provide an insight into the future development of antibacterial functional materials based on PDA.

Polydopamine antibacterial materials

Polyphenols are a class of ubiquitous compounds distributed in nature, with fascinating inherent biocompatible, bioadhesive, antioxidant, and antibacterial properties. The unique polyphenolic structures based on catechol or pyrogallol moieties allow for strong non-covalent interactions (e.g., multiple hydrogen bonding, electrostatic, and cation–π interactions) as well as covalent interactions (e.g., Michael addition/Schiff-base reaction, radical coupling reaction, and dynamic coordination interactions with boronate or metal ions). This review article provides an overview of the polyphenol-based scaffolds including the hydrogels, films, and nanofibers that have emerged from chemical and functional signatures during the past years. A full description of the structure–function relationships in terms of their utilization in wound healing, bone regeneration, and electroactive tissue engineering is also carefully discussed, which may pave the path towards the rational design and facile preparation of next-generation polyphenol scaffolds for tissue engineering applications.

Zhipeng Gu

Papers

Advances and Impact of Antioxidant Hydrogel in Chronic Wound Healing.

Regulating the absorption spectrum of polydopamine

Black Phosphorus Hydrogel Scaffolds Enhance Bone Regeneration via a Sustained Supply of Calcium-Free Phosphorus.

Polydopamine antibacterial materials

Polyphenol scaffolds in tissue engineering