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• A poly(ionic liquids) ionoadhesive (PIA) with high mechanical strength and excellent ionic conductivity was fabricated. • The PIAs exhibit outstanding environmental reliability. • The PIAs demonstrate a significant mechano-reinforced property during the repeated mechanical training. • The PIAs demonstrate extraordinary electrically detaching behavior and the detaching efficiency can reach over 90 %. Ionoadhesives hold great potentials for detachment and replacement of bonding components by virtue of the interfacial electrochemistry reactions of ion carriers, but previous ionoadhesives suffer from liquid leakage and conflict between mechanical properties and ionic conductivity. Here, a liquid-free and nanophase separated poly(ionic liquids) ionoadhesive (PIA) is designed through establishing multiple non-covalent interactions (NCIs) including weak ion–dipole interactions, moderate lithium bonds and strong electrostatic interactions. As a result, the physical crosslinked networks in PIAs are effectively strengthened that ensures the mechanical performances under static state; the breaking-reforming events of the multiple NCIs are beneficial for dissipating energy to resist external deformations that endows the PIAs with outstanding dynamic stability; the multiple NCIs also induce the orientation of nanophases that enables the PIAs to be reinforced via cyclic mechanical training. Benefiting from the high ionic conductivity, the PIAs exhibit extraordinary electrically detaching behavior under DC voltages since the occurrence of rapid interfacial electrochemistry reactions that facilitates the formation of gases and nanoparticles at the bonding interfaces. This work proposes a new rational design of electrically detachable ionoadhesives with excellent comprehensive performances that demonstrate great potentials in recycle and reuse of the bonding components and reduce the waste of industrial resources. [ABSTRACT FROM AUTHOR]

• Poly(ionic liquids) (PILs) functionalized with [MEDTA]2- were synthesized for NH 3 uptake. • The NH 3 capacity of PVIm-R8-MEDTA (M = Co, Cu, Ni, Mg, Zn) increased by 33–88 % compared with the conventional PILs. • The NH 3 was inserted into the coordinative bonds between carboxylate and metal ion and fixed by the hydrogen bonding with imidazolium cation. • The self-repairing [MEDTA]2- gives benift to the recovery of PVIm-R8-MEDTA under moisture and NH 3 atmosphere. MOFs have high adsorption performance of ammonia (NH 3) because of its porosity and abundant coordination sites, especially MOFs containing carboxylic acid ligands have emerged as effect NH 3 adsorbents. But, it's troublous for reversible ammonia adsorption for the strong metal-NH 3 coordination or the collapse of adsorbents. [MEDTA]2- is a very stable and classic carboxylic acid-containing complex, but there was no relevant report. Therefore, this work carried out the design and synthesis of PVIm-R8-MEDTA based on the use of the coordination structure of [MEDTA]2- and the stability of PILs' skeleton. The characterization indicated the [MEDTA]2- could be introduced into PILs successfully for the hydrogen bonding interactions with the imidazolium cation, and the obtained PVIm-R8-MEDTA presented enhanced NH 3 capacity (10.4–14.7 mmol/g) than their precursor PVIm-R8-Br (7.8 mmol/g). The mechanism of NH 3 adsorption was proposed by DFT calculation, spectroscopic method, and the calorimetric test, it indicated the NH 3 was fixed by imdazolium cation through hydrogen bonding and inserted into two of the carboxylate and metal bonds of [MEDTA]2-. Because of the multi-meshing coordination of [EDTA]4- and metal ions, the disconnected carboxylate ions could easily coordinate with metal ions again and repair the chelating structure of [MEDTA]2-, which caused the ammonia easily be desorbed. In the process of gas adsorption, there was no bonding breakage of the skeleton of PILs, which helped the PVIm-R8-MEDTA be recovered under moisture and NH 3 atmosphere. Thanks for the designability of PILs, such as the cationic structure, structure and size of cross-linking agent, the choice of complex anion and so on, it provides a new design idea and theoretical basis for efficient and reversible ammonia adsorption materials. [ABSTRACT FROM AUTHOR]

• Hydrogels exhibited excellent stretchability and low hysteresis. • Hydrogels have adhesion, conductivity and strong antibacterial activity. • This hydrogel was design for wound dressing and skin bioelectronics. • The hydrogel sensor could realize wireless real-time monitoring and remote alarm. With the increasing utilization of therapeutic materials in wound care and skin bioelectronics, there is growing requirements for multifunctional hydrogels for personal therapy and health management. However, the limited functionality, mechanical incompatibility, and impracticality of traditional dressings and skin bioelectronics greatly restrict their widespread use in clinical settings. Herein, we fabricate a cellulose nanofibers (CNFs)-reinforced poly(Ionic Liquids) (PILs) composite hydrogel (PAC x V y) which can be used as infected wound therapy and real-time reliable bioelectronic. The hydrogel showed an orderly interconnected cellular architecture with excellent stretchability, outstanding elasticity and low hysteresis. As a wound dressing, the hydrogel could provide the adhesion to seal wounds, biocompatibility and outstanding antibacterial activity, enabling the wound dressing to effectively inhibit bacterial growth and accelerate infected wound healing. ILs enables the hydrogel to have high conductivity, outstanding sensing performance and impressive temperature response. Therefore, the hydrogel may also work as novel flexible bioelectronics, which could accurately capture motion signals ranging from large strain to minute physiological signal, such as body movement, heart rate, pulse, and body temperature. Notably, a dual-channel remote clinical alarm system was fabricated by combining the hydrogel with tailor-made single-chip to wireless real-time monitoring of finger joint movement and temperature changes, which could establish a communication channel between patient and wounded and provide effective medical intervention timely. This line of research work sheds light on the hydrogel has significant implications for improving personal therapy and health management. [ABSTRACT FROM AUTHOR]

[Display omitted] • The hydrogels exhibit editable transparency, mechanical and drug loading properties. • The hydrogels achieve efficient and visualized drug release controlled by NIR or temperature. • The hydrogel sensors realize customized wound treatment and wireless state diagnosis. • The sensor arrays can identify strain, temperature and NIR light in 3D space and direction. Hydrogels with excellent flexibility, water retention, and biocompatibility are natural carriers for drug delivery. However, the poor drug compatibility seriously limits the practical application of traditional PNIPAM-based hydrogel. Herein, a photothermal regulated smart hydrogel was synthesized by introducing poly(ionic liquids) chain into the binary polymer chain. The temperature-induced hydrophilic-hydrophobic switchable poly(ionic liquids) chain endows the smart hydrogel with editable transparency, enabling intuitive visualization of drug loading and releasing capacity. The smart hydrogel could be used as NIR/temperature-controlled drug carrier to achieve efficient and visualized release (40.8 % drug release rate in 30 min). Besides, the smart hydrogel sensor showed excellent strain sensing sensitivity (gauge factor = 3.73), short response time (116 ms), high durability (1800 s at 20 % strain), and impressive temperature sensing sensitivity (TCR = -1.252 %/°C). Based on the excellent sensing performance and editable drug-delivery ability, the smart hydrogel was assembled into a dynamic wound management system to realize personalized wound treatment and wireless state diagnosis. The wireless sensor early warning system could realize wireless monitoring and state warning of joints (fingers, ankles, and elbows), exhibiting guiding significance for rehabilitation treatment. Moreover, the high-resolution sensor array composed of 5 × 5 smart hydrogels could accurately identify the strain, temperature and NIR light in three-dimensional space and direction. In short, the smart hydrogel provides an innovative solution to personalized wound diagnosis and assisted rehabilitation. [ABSTRACT FROM AUTHOR]

The hydrogel could exhibit fast antibacterial activity before biodegradation, and then the infected wound could be angiogenesis and healed after the hydrogel biodegradation. [Display omitted] • The halogen-free imidazolium poly(ionic liquids) were synthesized as antibacterial agents. • The hydrogel dressings contained halogen-free imidazolium poly(ionic liquids) and deferoxamine. • The hydrogel dressings exhibited fast antibacterial activity and angiogenesis. • The hydrogel dressings could programable repairing full-thickness skin defect wound. Full-thickness skin defect wound infection seriously threatens the life and health of patients. Highly efficient antibacterial activity and angiogenesis after injury are critical for the wound healing process. In this work, we first designed various of halogen-free imidazolium poly(ionic liquids) (PILs) as the antibacterial agents, and selected the highest efficient antibacterial PIL. Then, we fabricated hyaluronic acid/poly(ethylene glycol)/PILs semi interpenetrating polymer network (semi-IPN) wound dressings by Diels-Alder (DA) click reaction, and deferoxamine (DFO) which promoted angiogenesis was grafted into the hydrogel wound dressings. In vitro and in vivo assays respectively evaluated the fast antibacterial property of the hydrogels against Escherichia coli and Staphylococcus aureus at skin infected wound areas. With the hydrogels enzymatic degradation by hyaluronidase, the degradation solution could reduce inflammation, promote angiogenesis and wound healing due to the continuous releasing of DFO and PIL. The programable hydrogel degradation protocol provided a new strategy for rapid full-thickness skin defect wound healing in the clinic application. [ABSTRACT FROM AUTHOR]

[Display omitted] • The heterogeneous hollow polymerized ionic liquid spheres (PIL- x) were synthesized. • The hollow PIL- x with different anions possess hierarchical electronic structure. • Electronic potential junction can be formed by combining PIL- x and g-C 3 N 4. • The activity of hydrogen evolution was improved significantly. • The reaction activity can be tuned flexibly by changing the species of anions. Graphitic carbon nitride (g-C 3 N 4) has been considered as a promising organic semiconductor for photochemistry but under great challenges of severe recombination rate of photogenerated electron-hole pairs, the weak ability of light harvesting, and other inherent defects. Herein, uniformed hollow polymeric ionic liquid spheres with layer gradients of electron structure were developed innovatively combining with g-C 3 N 4 nanosheets driven by sonication and electrostatic forces. These two components can form a novel system due to the distinction of electron between poly(ionic liquids) (PILs) and g-C 3 N 4. The novel as-developed PILs- x loaded on the g-C 3 N 4 surface benefits the transfer and supplement of photoinduced electrons resulting from the effects of "electronic reservoir". Meanwhile, the light harvesting of the PILs- x /g-C 3 N 4 is also enhanced significantly. In addition, the "ion modulated effect" was studied by tuning the species of anion in PILs structure, achieving controllable regulation of photocatalytic activity. Benefiting from the above fascinating properties, the PILs- x /g-C 3 N 4 system exhibit a significantly enhanced hydrogen evolution efficiency with Pt as co-catalyst under visible light irradiation compared with the Pt/PCN. This study opens a new sight to strengthen the photocatalytic activity of g-C 3 N 4 by using functional hollow PILs with layer gradients of electron structure for various applications in energy and environmental fields. [ABSTRACT FROM AUTHOR]

• Semi-inter penetrate network hydrogels containing imidazolium poly(ionic liquids) were synthesized. • Imidazolium poly(ionic liquids) and montmorillonite clay could enhance the mechanical property of hydrogels. • Hydrogels exhibited fast antibacterial and anti-inflammatory properties. • Hydrogels were degraded rapidly, and the degrading solution promote cell migration and proliferation. The development of treatment of wound healing cannot meet clinical requirements owing to the complex bacteria-infection and inflammatory reaction. It is necessary to develop wound dressings that are fast antibacterial property, anti-inflammation and promoting cell migration and proliferation for shortening wound healing period. In this work, we first synthesized two poly(ionic liquids) (PILs): poly(1-ethyl-3-vinylimidazolium furan-2-carboxylate) (PEIF) and poly(1-butyl-3-vinylimidazolium furan-2-carboxylate) (PBIF). The PILs were then mixed with 5 wt% montmorillonite (MMT) clay and 2-furfurylamine-modified hyaluronic acid (HAF), and chemically crosslinked with four-arm maleimide-polyethylene glycol (Mal 4 PEG) to form degradable semi-inter penetrate network (semi-IPN) hydrogels. In vitro assays demonstrated that the synthesized semi-IPN hydrogels exhibited high antibacterial activities against Escherichia coli and Staphylococcus aureus due to the high antibacterial activity of PILs. Furthermore, the semi-IPN hydrogel could be quickly degraded, and the PILs exhibited high anti-inflammatory activities when they were released from degraded hydrogels. The degradation solutions of hydrogels contained glycosaminoglycan, which was beneficial to cell proliferation and migration. The in vivo anti-infection results further demonstrated that the semi-IPN hydrogels could kill S. aureus and accelerate the healing of infected wounds. [ABSTRACT FROM AUTHOR]