Solvent-Triggered, Ultra-Adhesive, Conductive, and Biocompatible Transition Gels for Wearable Devices.

The development of robust adhesive, conductive, and flexible materials has garnered significant attention in the realm of human-machine interface and electronic devices. Conventional preparation methods to achieve these exceptional properties rely on incorporating highly polar raw materials, multiple components, or solvents. However, the overexposure of functional groups and the inherent toxicity of organic solvents often render gels non-stick or potentially biocompatible making them unsuitable for human-contact devices. In this study, a straightforward three-step strategy is devised for preparing responsive adhesive gels without complex components. Structurally conductive poly(N-(2-hydroxyethyl)-acrylamide-co-p-styrene sulfonate hydrate) (PHEAA-NaSS) gels are synthesized by integrating ionic and hydrophilic networks with distinct solvent effects. Initially, the in-suit formed PHEAA-NaSS networks are activated by dimethyl sulfoxide, which substantially increases intramolecular hydrogen bonding and enhances the matrix stretchability and interfacial adhesion. Subsequently, ethanol exchange reduced solvent impact and led to a compact network that limited surface exposure of ionic and hydrophilic groups, resulting in nonstick, robust for convenient storage. Finally, upon contacting with water, the network demonstrates rehydration, resulting in favorable adhesion, biocompatibility, and conductivity. The proposed PHEAA-NaSS/W gels can stably and reliably capture joint motion and electrophysiological signals. Furthermore, this uncomplicated gel preparation method is also applicable to other electrolyte monomers.

Environmentally Adaptable Organo-Ionic Gel-Based Electrodes for Real-Time On-Skin Electrocardiography Monitoring.

On-skin personal electrocardiography (ECG) devices, which can monitor real-time cardiac autonomic changes, have been widely applied to predict cardiac diseases and save lives. However, current interface electrodes fail to be unconditionally and universally applicable, often losing their efficiency and functionality under harsh atmospheric conditions (e.g., underwater, abnormal temperature, and humidity). Herein, an environmentally adaptable organo-ionic gel-based electrode (OIGE) is developed with a facile one-pot synthesis of highly conductive choline-based ionic liquid ([DMAEA-Q] [TFSI], I.L.) and monomers (2,2,2-trifluoroethyl acrylate (TFEA) and N-hydroxyethyl acrylamide (HEAA). In virtue of inherent conductivity, self-responsive hydrophobic barriers, dual-solvent effect, and multiple interfacial interactions, this OIGE features distinct sweat and water-resistance, anti-freezing and anti-dehydration properties with strong adhesiveness and electrical stability under all kinds of circumstances. In contrast to the dysfunction of commercial gel electrodes (CGEs), this OIGE with stronger adhesion as well as skin tolerability can realize a real-time and accurate collection of ECG signals under multiple extreme conditions, including aquatic environments (sweat and underwater), cryogenic (<-20°C) and arid (dehydration) environments. Therefore, the OIGE shows great prospects in diagnosing cardiovascular diseases and paves new horizons for multi-harsh environmental personalized healthcare.

A biomimetic and bioactive scaffold with intelligently pulsatile teriparatide delivery for local and systemic osteoporosis regeneration.

Osteoporosis is one of the most disabling consequences of aging, osteoporotic fractures and higher risk of the subsequent fractures leading to substantial disability and deaths, indicating both local fractures healing and the early anti-osteoporosis therapy are of great significance. Teriparatide is strong bone formation promoter effective in treating osteoporosis, while side effects limit clinical applications. Traditional drug delivery is lack of sensitive and short-term release, finding a new non-invasive and easily controllable drug delivery to not only repair the local fractures but also improve total bone mass has remained a great challenge. Thus, bioinspired by the natural bone components, we develop appropriate interactions between inorganic biological scaffolds and organic drug molecules, achieving both loaded with the teriparatide in the scaffold and capable of releasing on demand. Herein, biomimetic bone microstructure of mesoporous bioglass, a near-infrared ray triggered switch, thermosensitive liposomes based on a valve, and polydopamine coated as a heater is developed rationally for osteoporotic bone regeneration. Teriparatide is pulsatile released from intelligent delivery, not only rejuvenating osteoporotic bone defect, but also presenting strong systemic anti-osteoporosis therapy. This biomimetic bone carrying novel drug delivery platform is well worth expecting to be a new promising strategy and clinically commercialized to help patients survive from the osteoporotic fracture.

Ionic interaction-driven switchable bactericidal surfaces.

Bacteria in the external environment inevitably invade the wound and subsequently colonize the wound surface during surgery and biomedical operations, which slows down the process of wound healing and tissue repair; this poses a significant threat to human health. Therefore, the development of an intelligent antibacterial surface has become the focus of research in the field of antimicrobial strategies, which has important social and economic significance. Here, we present a simple approach of producing an ionic interaction-driven anionic activation substratum which is then functionalized with cationic molecules through coulombic interactional immobilization. The switchable multifunctional antibacterial surface can decrease bacterial attachment and inactivate the attached microorganisms, thus overcoming the conventional challenge for antibacterial surfaces. Briefly, poly (3-sulfopropyl methacrylate potassium salt) (PSPMA) brushes were constructed by surface-initiated atom transfer radical polymerization on silicon or cotton fabric substrates, and a positive-charged component, namely lysozyme (LYZ), hexadecyl trimethyl ammonium bromide (CTAB) or chitosan (CS), was loaded on negative-charged sulfonate groups through electrostatic interactions. The resultant brush-grafted surfaces exhibited more than ∼95.5% bactericidal efficacy and ∼92.8% release rate after the introduction of an adequate amount of contra-ions (1.0 M; Na+ & Cl-) against both Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus, thus achieving a regenerated surface through the cyclic process of "assembly-dissociation". Smart cotton fabric (Fabric-PSPMA/LYZ and Fabric-PSPMA/CS) surfaces were constructed, which were found to promote wound epidermal tissue regeneration with a higher efficiency after 7-day in vivo studies. This ionic interaction-driven method used in the present work is simple and can reversibly renew antibacterial surfaces, which will help in the wider utilization of switchable antibacterial materials with a more ecologic and economic significance. STATEMENT OF SIGNIFICANCE: Smart antibacterial surfaces with renewable characteristics have attracted considerable interests over the past few years. Here, we used ionic interaction-driven force to manipulate dynamic conformational changes in PSPMA surface brushes, accompanied by highly switchable bacteria killing and bacteria releasing behaviors. Different cationic molecules were also designed for assembly/dissociation on the PSPMA-modified surfaces, and the essential parameters, including chemical structures, molecular weight, and cationic charge density, were investigated. With the refined structural combinations and the balance of bacteria killing/bacteria releasing behaviors, smart cotton fabrics (e.g., Fabric-PSPMA/lysozyme and Fabric-PSPMA/chitosan) were designed that could promote wound healing and tissue repair. These results contribute to the fundamental understanding of a switchable cationic-anionic pair design and the corresponding practical, renewable, highly antibacterial fabric.

Cationic peptide-based salt-responsive antibacterial hydrogel dressings for wound healing.

Development of biological dressings has received widespread attentions due to their good breathability, biocompatibility, wettability, and the ability to absorb wound exudate without sticking to the wound. However, current proposed antibacterial hydrogels are limited antibacterial ability, short service life and insufficient biocompatibility, which are still challenging to address intricate practical applications. Here we develop a cationic peptide-based, salt-responsive hydrogel dressing with triple functions of antifouling, bactericidal, and bacterial release by combining ε-poly-l-lysine, poly(ethylene glycol) diglycidyl ether, and poly(DVBAPS-co-GMA) via a one-pot method. These designed hydrogels enabled to further quaternize to enhance antibacterial property due to the presence of amine residues. The resultant hydrogels present good antibacterial activity (>90%), biocompatibility, cell proliferation efficacy (~400%) and adhesiveness. Through in vivo and in vitro antibacterial capability tests, it is also found that hydrogels have good antifouling and sterilization capabilities, and the sterilization rate could reach up to ~96%. In addition, ~94% of the attached bacterial can be released after saline/water switching for several cycles. Taken together, the designed multiple antibacterial dressing prolongs the lifespan relying on reversible salt-responsive release and meet special requirements for wound healing. This work not only provides a platform to highlight its promising potentials in wound management but also gives a custom strategy to biomedical applications.

Retraction Notice to: Application of Inorganic Nanocomposite Hydrogels in Bone Tissue Engineering.

[This retracts the article DOI: 10.1016/j.isci.2020.101845.].

Host-Guest Interaction-Mediated Photo/Temperature Dual-Controlled Antibacterial Surfaces.

Development of smart switchable surfaces to solve the inevitable bacteria attachment and colonization has attracted much attention; however, it proves very challenging to achieve on-demand regeneration for noncontaminated surfaces. We herein report a smart, host-guest interaction-mediated photo/temperature dual-controlled antibacterial surface, topologically combining stimuli-responsive polymers with nanobactericide. From the point of view of long-chain polymer design, the peculiar hydration layer generated by hydrophilic poly(2-hydroxyethyl methacrylate) (polyHEMA) segments severs the route of initial bacterial attachment and subsequent proliferation, while the synergistic effect on chain conformation transformation poly(N-isopropylacrylamide) (polyNIPAM) and guest complex dissociation azobenzene/cyclodextrin (Azo/CD) complex greatly promotes the on-demand bacterial release in response to the switch of temperature and UV light. Therefore, the resulting surface exhibits triple successive antimicrobial functions simultaneously: (i) resists ∼84.9% of initial bacterial attachment, (ii) kills ∼93.2% of inevitable bacteria attack, and (iii) releases over 94.9% of killed bacteria even after three cycles. The detailed results not only present a potential and promising strategy to develop renewable antibacterial surfaces with successive antimicrobial functions but also contribute a new antimicrobial platform to biomedical or surgical applications.

Application of Inorganic Nanocomposite Hydrogels in Bone Tissue Engineering.

Bone defects caused by trauma and surgery are common clinical problems encountered by orthopedic surgeons. Thus, a hard-textured, natural-like biomaterial that enables encapsulated cells to obtain the much-needed biophysical stimulation and produce functional bone tissue is needed. Incorporating nanomaterials into cell-laden hydrogels is a straightforward tactic for producing tissue engineering structures that integrate perfectly with the body and for tailoring the material characteristics of hydrogels without hindering nutrient exchange with the surroundings. In this review, recent developments in inorganic nanocomposite hydrogels for bone tissue engineering that are of vital importance but have not yet been comprehensively reviewed are summarized.

Eco-friendly development of an ultrasmall IONP-loaded nanoplatform for bimodal imaging-guided cancer theranostics.

Success in disease therapy depends on precision medicines, where development of formulations with diagnostic and therapeutic functions is quite important. In this study, multifunctional theranostics based on a magnetic graphene oxide (GO) nanohybrid (GIPD) has been developed for magnetic resonance (MR) imaging-guided chemo-photothermal therapy of cancer. The GIPD is endowed with T1/T2 MR imaging capacity via precipitation of small-sized IONP nanoparticles (8.25 ± 2.25 nm) on GO nanosheets through a mild friendly way (60 °C for 1 h, no organic solvent). The obtained nanocomposite is then non-covalently decorated with phosphine oxide polyethylene glycol to improve biosafety. The final nanohybrid effectively loads doxorubicin as the model chemotherapeutic drug and is found to have in vivo T1/T2 MR bimodal imaging functions. Both the in vitro and in vivo results demonstrate that the GO-based nanoplatform displays a good remote photothermal effect, which can damage the dense shell of solid tumor tissue, thereby facilitating the delivery of anticancer drugs into tumor cells. Therefore, this theranostic nanoplatform enables a potent combined chemo-photothermal anticancer efficacy, holding great potential for exploitation of precision cancer therapy.

A novel strategy for tumor therapy: targeted, PAA-functionalized nano-hydroxyapatite nanomedicine.

The rapid development of nanotechnology has provided new strategies for the treatment of tumors. Nano-scale hydroxyapatite (HAP), as the main component of hard tissues in humans and vertebrates, have been found to specifically inhibit tumor cells. However, achieving controllable synthesis of HAP and endowing it with cancer cell-targeting properties remain enormous challenges. To solve this problem, we developed polyacrylic acid-coordinated hydroxyapatite nanoparticles (HAP-PAA) and further chemically grafted them with folic acid (HAP-PAA-FA) for cancer treatment in this study. The nucleation sites and steric hindrance provided by the PAA greatly inhibited the agglomeration of the nanoparticles, and at the same time, the excess functional groups further modified the surface of nanoparticles to achieve targeting efficiency. The spherical, low-crystallinity HAP-PAA nanoparticles exhibited good tumor cell lethality. After grafting the nanoparticles with folic acid for molecular targeting, their cellular uptake and specific killing ability of tumor cells were further enhanced. The HAP-PAA-FA nanoparticle system exerted a regulatory effect on the tumor microenvironment and had good biological safety. All the above results indicate that this research will broaden the application of hydroxyapatite in tumor treatment.

Bimetallic Metal-Organic Framework-Derived Carbon Nanotube-Based Frameworks for Enhanced Capacitive Deionization and Zn-Air Battery.

Carbon-based materials have attracted intensive attentions for a wide range of energy and environment-related applications. Energy storage/conversion devices with improved performance have been achieved by utilization of metal-organic-framework (MOF)-derived carbon structures as active materials in recent years. However, the effects of MOF precursors on the performance of derived carbon materials are rarely investigated. Here, we report that the incorporation of small amount of Fe or Ni in Co-based MOFs leads to a significant enhancement for the derived carbon nanotube-based frameworks (CNTFs) in Na+/Cl- ion electrosorption. Further investigation revealed the enhanced performance can be attributed to the improved specific surface area, electrical conductivity, and electrochemical activity. Notably, the CoFe-CNTF derived from bimetallic CoFe-MOFs achieves a high ion adsorption capacity of 37.0 mg g-1, superior to most of recently reported carbon-based materials. Furthermore, the CoFe-CNTF also demonstrates high catalytic activity toward oxygen evolution reaction (OER) with a Tafel slope of 87.7 mV dec-1. After combination with three-dimensional graphene foam (3DG), the resultant CoFe-CNTF-coated 3DG is used as air-cathode to fabricate a flexible all-solid-state Zn-air battery, which exhibits a high open circuit potential of 1.455 V. Importantly, the fabricated flexible battery can light a light-emitting diode (LED) even when it is bent. This work provides new insights into designs of high-performance and flexible electrode based on MOF-derived materials.