Wearable and implantable bioelectronics are receiving a great deal of attention because they offer huge promise in personalized healthcare. Currently available bioelectronics generally rely on external aids to form an attachment to the human body, which leads to unstable performance in practical applications. Self‐adhesive bioelectronics are highly desirable for ameliorating these concerns by offering reliable and conformal contact with tissue, and stability and fidelity in the signal detection. However, achieving adequate and long‐term self‐adhesion to soft and wet biological tissues has been a daunting challenge. Recently, mussel‐inspired hydrogels have emerged as promising candidates for the design of self‐adhesive bioelectronics. In addition to self‐adhesiveness, the mussel‐inspired chemistry offers a unique pathway for integrating multiple functional properties to all‐in‐one bioelectronic devices, which have great implications for healthcare applications. In this report, the recent progress in the area of mussel‐inspired self‐adhesive bioelectronics is highlighted by specifically discussing: 1) adhesion mechanism of mussels, 2) mussel‐inspired hydrogels with long‐term and repeatable adhesion, 3) the recent advance in development of hydrogel bioelectronics by reconciling self‐adhesiveness and additional properties including conductivity, toughness, transparency, self‐healing, antibacterial properties, and tolerance to extreme environment, and 4) the challenges and prospects for the future design of the mussel‐inspired self‐adhesive bioelectronics.

2D conductive nanosheets are central to electronic applications because of their large surface areas and excellent electronic properties. However, tuning the multifunctions and hydrophilicity of conductive nanosheets are still challenging. Herein, a green strategy is developed for fabricating conductive, redox-active, water-soluble nanosheets via the self-assembly of poly(3,4-ethylenedioxythiophene) (PEDOT) on the polydopamine-reduced and sulfonated graphene oxide (PSGO) template. The conductivity and hydrophilicity of nanosheets are highly improved by PSGO. The nanosheets are redox active due to the abundant catechol groups and can be used as versatile nanofillers in developing conductive and adhesive hydrogels. The nanosheets create a mussel-inspired redox environment inside the hydrogel networks and endow the hydrogel with long-term and repeatable adhesiveness. This hydrogel is biocompatible and can be implanted for biosignals detection in vivo. This mussel-inspired strategy for assembling 2D nanosheets can be adapted for producing diverse multifunctional nanomaterials, with various potential applications in bioelectronics.because of their fascinating properties such as large surface areas, numerous active sites, and high conductivity and mechanical strength. [4] In particular, the emerging class of redox-active 2D conductive nanosheets such as covalent organic framework [5] and redox-active heteroatomloaded carbon nanosheets [6] has been used in various areas, e.g., catalysis, solar cells, photochemical water splitting, organic rechargeable battery cathodes, and bioelectronics. The common approach of fabricating conductive nanosheets via mechanical exfoliation lacks effective function tunability. Incorporation of inorganic redox couples such as transition-metal ions has frequently been used to make conductive nanosheets redox active. [7] However, these redox couples often involve toxic and precious-metal ions, and this hinders their biomedical applications. There is therefore an urgent need to develop green and costeffective approaches to fabricating biocompatible, redox-active, and conductive nanosheets for future bioelectronic and biomedical applications.Composites of conductive nanosheets and hydrogels are considered to be promising candidates for use in next-generation soft and flexible bioelectronics. [8] Poly(3,4-ethylenedioxythiophene) (PEDOT) is an ideal conductive material for flexible electronics because of its high electrical conductivity and excellent chemical stability. [9] However, because of the hydrophobicity and intrinsic chemical structure of PEDOT, the production of PEDOT nanosheets and their uniform dispersion in a hydrogel matrix is challenging. In addition, interfacial adhesion between the hydrogel and tissues is of critical importance, especially for electronic skin and implantable bioelectrode. [10] It is desire to develop flexible and tissue-adhesive bioelectronics so that they can tightly integrate with surrounding tissues. Recently, adhesive hydrogels based on mussel-inspired c...

Tough and conductive hydrogels are the promising materials for various applications. However, fabrication of these hydrogels at room or low temperatures, without external stimuli, is a challenge. Herein, a novel dual self-catalytic system composed of a variety of metal ions and catechol-based molecules was developed to efficiently trigger the free-radical polymerization of tough, conductive, transparent, and self-healing hydrogels at low temperature without any external stimuli. Ferric ions (Fe3+) and dopamine (DA) were chosen as model compounds, which form stable redox pairs that act as a dual self-catalytic system to activate ammonium persulfate to generate free radicals. Consequently, the radicals could rapidly trigger the hydrogel self-gelation at low temperatures (6 °C) within 5 s. The dual self-catalytic system opens up a facile route to synthesize multifunctional hydrogels at mild conditions for a broad range of applications, especially in tissue engineering and wearable electronics.

Research on incorporation of both growth factors and silver (Ag) into hydroxyapatite (HA) coatings on metallic implant surfaces for enhancing osteoinductivity and antibacterial properties is a challenging work. Generally, Ag nanoparticles are easy to agglomerate and lead to a large increase in local Ag concentration, which could potentially affect cell activity. On the other hand, growth factors immobilization requires mild processing conditions so as to maintain their activities. In this study, bone morphology protein-2 (BMP-2) and Ag nanoparticle contained HA coatings were prepared on Ti surfaces by combining electrochemical deposition (ED) of Ag and electrostatic immobilization of BMP-2. During the ED process, chitosan (CS) was selected as the stabilizing agent to chelate Ag ions and generate Ag nanoparticles that are uniformly distributed in the coatings. CS also reduces Ag toxicity while retaining its antibacterial activity. Afterwards, a BMP/heparin solution was absorbed on the CS/Ag/HA coatings. Consequently, BMP-2 was immobilized on the coatings by the electrostatic attraction between CS, heparin, and BMP-2. Sustained release of BMP-2 and Ag ions from HA coatings was successfully demonstrated for a long period. Results of antibacterial tests indicate that the CS/Ag/HA coatings have high antibacterial properties against both Staphylococcus epidermidis and Escherichia coli. Osteoblasts (OB) culture reveals that the CS/Ag/HA coatings exhibit good biocompatibility. Bone marrow stromal cells (BMSCs) culture indicates that the BMP/CS/Ag/HA coatings have good osteoinductivity and promote the differentiation of BMSCs. Ti bars with BMP/CS/Ag/HA coatings were implanted into the femur of rabbits to evaluate the osteoinductivity of the coatings. Results indicate that BMP/CS/Ag/HA coatings favor bone formation in vivo. In summary, this study presents a convenient and effective method for the incorporation of growth factors and antibacterial agents into HA coatings. This method can be utilized to modify a variety of metallic implant surfaces.

Ideal epidermal bioelectronics can be used not only for long‐term detection of physiological signals for disease diagnosis but also for chronic disease treatment. Silk, an animal‐derived fiber with good biocompatibility and skin‐affinity, is widely used in flexible bioelectronics. However, silk fibers are insulating. In this study, ultralong conductive silk microfibers (mSFs) are fabricated by extracting mSF from raw silk using a bioinspired extraction‐protection process with the assistance of polydopamine, followed by deposition of poly(3,4‐ethylenedioxythiophene) (PEDOT) on its surface. The conductive mSFs are produced and used to fabricate a conductive flexible silk fibroin patch, which is used as a conformable bioelectronic for monitoring physiological signals. In addition, as the conductive mSF possessed anti‐oxidative activity, the patch exhibits excellent performance in chronic diabetic wound healing by reducing inflammation and regulating oxidative stress. Thus, this bioinspired strategy produces conductive silk fibers that can be used as biocompatible building blocks, opening new avenues for employing passive silk as an active component in the design of epidermal wound repair biomaterials and next‐generation flexible epidermal bioelectronics.

Adhesive hydrogels have broad applications ranging from tissue engineering to bioelectronics; however, fabricating adhesive hydrogels with multiple functions remains a challenge. In this study, a mussel-inspired tannic acid chelated-Ag (TA-Ag) nanozyme with peroxidase (POD)-like activity was designed by the in situ reduction of ultrasmall Ag nanoparticles (NPs) with TA. The ultrasmall TA-Ag nanozyme exhibited high catalytic activity to induce hydrogel self-setting without external aid. The nanozyme retained abundant phenolic hydroxyl groups and maintained the dynamic redox balance of phenol-quinone, providing the hydrogels with long-term and repeatable adhesiveness, similar to the adhesion of mussels. The phenolic hydroxyl groups also afforded uniform distribution of the nanozyme in the hydrogel network, thereby improving its mechanical properties and conductivity. Furthermore, the nanozyme endowed the hydrogel with antibacterial activity through synergistic effects of the reactive oxygen species generated via POD-like catalytic reactions and the intrinsic bactericidal activity of Ag. Owing to these advantages, the ultrasmall TA-Ag nanozyme-catalyzed hydrogel could be effectively used as an adhesive, antibacterial, and implantable bioelectrode to detect bio-signals, and as a wound dressing to accelerate tissue regeneration while preventing infection. Therefore, this study provides a promising approach for the fabrication of adhesive hydrogel bioelectronics with multiple functions via mussel-inspired nanozyme catalysis.

Biomimetic calcium phosphate mineralized graphene oxide/chitosan (GO/CS) scaffolds with hierarchical structures were developed. First, GO/CS scaffolds with large micropores (∼300 μm) showed high mechanical strength due to the electrostatic interaction between the oxygen-containing functional groups of GO and the amine groups of CS. Second, octacalcuim phosphate (OCP) with porous structures (∼1 μm) was biomimetically mineralized on the surfaces of the GO/CS scaffolds (OCP-GO/CS). The hierarchical microporous structures of OCP-GO/CS scaffolds provide a suitable environment for cell adhesion and growth. The scaffolds have exceptional adsorbability of nanoparticles. Bone morphogenetic protein-2 (BMP-2)-encapsulated bovine serum albumin (BSA) nanoparticles and Ag nanoparticles (Ag-NPs) were adsorbed in the scaffolds for enhancement of osteoinductivity and antibacterial properties, respectively. Antibacterial tests showed that the scaffolds exhibited high antibacterial properties against both Escherichia coli and Staphylococcus epidermidis. In vitro and in vivo experiments revealed that the scaffolds have good biocompatibility, enhanced bone marrow stromal cells proliferation and differentiation, and induced bone tissue regeneration. Thus, the biomimetic OCP-GO/CS scaffolds with immobilized growth factors and antibacterial agents might be excellent candidates for bone tissue engineering.

Conductive polymers (CPs) are generally insoluble, and developing hydrophilic CPs is significant to broaden the applications of CPs. In this work, a mussel-inspired strategy was proposed to construct hydrophilic CP nanoparticles (CP NPs), while endowing the CP NPs with redox activity and biocompatibility. This is a universal strategy applicable for a series of CPs, including polyaniline, polypyrrole, and poly(3,4-ethylenedioxythiophene). The catechol/quinone contained sulfonated lignin (LS) was doped into various CPs to form CP/LS NPs with hydrophilicity, conductivity, and redox activity. These CP/LS NPs were used as versatile nanofillers to prepare the conductive hydrogels with long-term adhesiveness. The CP/LS NPs-incorporated hydrogels have a good conductivity because of the uniform distribution of the hydrophilic NPs in the hydrogel network, forming a well-connected electric path. The hydrogel exhibits long-term adhesiveness, which is attributed to the mussel-inspired dynamic redox balance of catechol/quinone groups on the CP/LS NPs. This conductive and adhesive hydrogel shows good electroactivity and biocompatibility and therefore has broad applications in electrostimulation of tissue regeneration and implantable bioelectronics.