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Compared with other types of sensors, capacitive flexible pressure sensors (CFPS), with low sensitivity, are more susceptible to environmental changes. It is still a considerable challenge to achieve high sensitivity, excellent mechanical properties and long-time structural stability simultaneously. Targeting the aforementioned issues, herein, Ti3C2 (MXene) with high dielectric constant was firstly chemically modified with a poly(ionic liquid) (PIL) via surface-initiated ATRP, and then combined with a porous polyurethane foam (PUF) 3D network structure via a one-step blending foaming method. Thanks to the organic-inorganic hybrid network based on the PU/MXene porous structures and the uniformly distributed micro-capacitor structure provided by MXene@PIL, the mechanical properties, structural stability, flame retardancy and dielectric properties of the composite foam were all significantly enhanced. When the content of MXene@PIL was 10%, the sensitivity of CFPS based on this dielectric were 17.1, 5.2, and 2.5/KPa in the pressure ranges of 0-1 KPa, 1-12 KPa and 12-100 KPa, respectively. In addition, the sensor showed the response and recovery times of 88 and 82 ms under a low pressure of 355 Pa. The light, flexible sensor prepared in this work is expected to be used in wearable devices to monitor physiological signals, and it should also be a good candidate for the next generation of man-machine interface characterization devices. [ABSTRACT FROM AUTHOR]

Metal‐to‐metal adhesives are vital across diverse sectors including automotive, aerospace, and industrial assembly. However, traditional adhesion detection methods are mainly based on the fracture mechanism, posing challenges for nondestructive detection. Here, a nondestructive method that leverages electrical signals to monitor the adhesion state of metal interfaces in real‐time is presented. The approach utilizes detectable adhesives (DA) synthesized from poly(ionic liquid) (PIL), which not only exhibit robust adhesion properties (4.9 MPa) but also function as ionic conductors. By correlating changes in capacitance and resistance with the adhesive state, the method allows for in situ monitoring of the curing process, prediction of adhesion strength, and early detection of potential failures. This dual‐sensing capability, combining electrical and mechanical aspects, enhances understanding of adhesive behavior in diverse conditions, presenting a fresh approach for digitally transforming adhesive technologies. [ABSTRACT FROM AUTHOR]

In this study, we report the synthesis of 3‐, 4‐, and 6‐arm star poly(ionic liquid)s (PILs) (specifically, star poly(vinylbenzyl methylimidazolium bis(trifluoromethane)sulfonimide) (poly(VBMIm‐TFSI))) via reversible addition‐fragmentation chain transfer (RAFT) polymerization with a core‐first approach, followed by quaternization and anion exchange. The impact of star polymer architecture on properties was explored by measuring the thermal, mechanical, and ion transport properties of each star PIL compared to those of an analogous linear PIL. The star PILs exhibited up to 2‐fold higher ionic conductivity, 150% higher elastic modulus, and 465% higher ultimate tensile strength compared to the analogous linear PIL. The Williams‐Landel‐Ferry (WLF) equation was employed to explore the effect of increased free volume on the improved ion transport properties of the star PILs. These results highlight the impact of star polymer architecture on PILs and star PILs as promising materials for electrochemical energy devices. [ABSTRACT FROM AUTHOR]

Ionic covalent organic frameworks (iCOFs) are crystalline materials with stable porous structures. They hold great potential for ion transport, particularly as solid‐state electrolytes (SSEs) for all‐solid‐state lithium metal batteries (ASSLMBs). However, achieving an ionic conductivity of over 10−3 S cm−1 at room temperature using pure‐iCOF‐based SSEs, even adding additives such as lithium salts, is challenging as the voids work as strong resistances. Thus, highly conductive iCOFs typically require quasi‐solid‐state configurations with organic solvents or plasticizers. In this study, composites comprising iCOFs and poly(ionic liquid) (PIL) are prepared to make all‐solid‐state iCOFs electrolytes with an exceptional ionic conductivity up to 1.50 × 10−3 S cm−1 and a high Li+ transference number of > 0.80 at room temperature. Combined experimental and computational studies show that the co‐coordination and competitive coordination mechanism established between the PIL, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and iCOFs enabled rapid Li+ transport while restricting TFSI− movement. ASSLMB cells, made of composite SSEs and LiFePO4 composite cathode, demonstrate an initial discharge capacity of 141.5 mAh g−1 at 1C and r.t., with an impressive capacity retention of 87% up to 800 cycles. Overall, this work presents a breakthrough approach for developing advanced SSEs for next‐generation high‐energy‐density ASSLMBs. [ABSTRACT FROM AUTHOR]

The development of efficient heterogeneous catalysts for upgrading CO2, a greenhouse gas, and glycerol (Gly), an untapped biomass resource, into glycerol carbonate (GC) remains a challenge. Herein, 1,8‐diazabicyclo[5.4.0] undec–7–ene (DBU)–based poly (ionic liquid)s (PILs) were constructed for the one–pot synthesis of GC from CO2, Gly, and propylene oxide. Among them, P−DVB−DBUVBI–1 exhibited the best catalytic performance, achieving a GC yield of 90 % under optimal reaction conditions (100 °C, 6 h). The PIL catalyst was easily recovered and reused, as demonstrated by stable activity over five cycles. Density functional theory calculations showed that owing the strong positive charge delocalization ability of DBU onium, DBU–based PILs exhibit high nucleophilicity, which is the key to their efficient catalytic performance in the one–pot reaction. [ABSTRACT FROM AUTHOR]

The escalating spread of drug‐resistant bacteria and viruses is a grave concern for global health. Nucleic acids dominate the drug‐resistance and transmission of pathogenic microbes. Here, imidazolium‐type poly(ionic liquid)/porphyrin (PIL‐P) based electrospun nanofibrous membrane and its cerium (IV) ion complex (PIL‐P‐Ce) are developed. The obtained PIL‐P‐Ce membrane exhibits high and stable efficiency in eradicating various microorganisms (bacteria, fungi, and viruses) and decomposing microbial antibiotic resistance genes and viral nucleic acids under light. The nuclease‐mimetic and photocatalytic mechanisms of the PIL‐P‐Ce are elucidated. Co‐infection wound models in mice with methicillin‐resistant S. aureus and hepatitis B virus demonstrate that PIL‐P‐Ce integrate the triple effects of cationic polymer, photocatalysis, and nuclease‐mimetic activities. As revealed by proteomic analysis, PIL‐P‐Ce shows minimal phototoxicity to normal tissues. Hence, PIL‐P‐Ce has potential as a "green" wound dressing to curb the spread of drug‐resistant bacteria and viruses in clinical settings. [ABSTRACT FROM AUTHOR]

Though polyvinylidene fluoride (PVDF) is widely‐used binder for conventional lithium‐sulfur (Li–S) batteries, it still encounters challenges of severe electrode fracture involved by drastic volume change upon repeating cycling, and lack of extended‐functions like trapping dissolved polysulfides and smoothing Li+ transfer. Herein, a methodology of grafting sulfophilic hydrogen‐bond donor and lithiophilic hydrogen‐bond acceptor to the polymer binder (named as PIL), function as gear teethes and tooth spaces, is reported. When cracks occur, the engaged gears driven by dynamic hydrogen bonds are separated, which are spontaneously reformed owing to the automatic meshing of gears, and thus accelerate the healing of cracks. At the molecular level, the synergetic effect of sulfophilic hydrogen‐bond donor and lithiophilic hydrogen‐bond acceptor enables polysulfides immobilization through “push‐pull effect”, facilitating the subsequent redox kinetics. Accordingly, the cross‐link network of hydrogen bonds endows the elaborated designed polymer binder with strong adhesive strength and rapid Li+ migration. Attributed to these beneficial properties, the PIL‐based sulfur cathode exhibits excellent rate performance and superior cycling durability (an ultralow capacity fading rate of 0.062% per cycle over 800 cycles at 2 C). Even with high sulfur loading of 9.27 mg cm−2, a high areal capacity of 8.71 mAh cm−2 can be achieved, verifying its potential application. [ABSTRACT FROM AUTHOR]

The enzyme carbonic anhydrase (CA) has gainned considerable attention from the literature and the industry in the context of CO2 capture. CA immobilization in gas-liquid membrane contactors, and more specifically, on poly(ionic liquid) (PIL) composite membranes has been demonstrated to be a potential strategy to facilitate its industrial implementation. These membranes were comprised of a PIL layer coating on a porous hydrophobic polymeric support. In this work, the composition of the PIL layer was tuned by anion exchange to yield a variety of enzyme carriers. The following anions were compared: bromide [Br], acetate [Ac], tetrafluoroborate [BF4], and bis(trifluoromethylsulfonyl)imide [NTf2]. The surface morphology, chemistry, and properties of these composite membranes were characterized by SEM, EDX, ATR-FTIR, and water contact angle. The activity of the different biocatalytic composite membranes was determined by the p-nitrophenyl acetate hydrolysis model reaction. It was found that the anion exchange salts had a detrimental effect on the immobilized enzyme activity. In light of these results, the enzyme immobilization step was conducted after anion exchange. The resulting biocatalytic membranes displayed slight differences in immobilized enzyme activities and thermal stabilities following the order [Br]>[BF4]>[Ac]>[NTf2] and [BF4]>[Br]≈[Ac]>[NTf2], respectively. The differences were more pronounced and detrimental for the most hydrophobic anion, [NTf2]. Parallel trends were noted when the membranes were tested for CO2 absorption in a gas-liquid membrane contactor set-up suggesting that the CO2 mass transfer is strongly influenced by the activity of the immobilized enzymes. In addition, the effect of the absorption conditions, i.e., solvent flow rate, solvent saturation, and solvent concentration were evaluated. Under the best conditions, the novel biocatalytic membranes outperformed the commercial PVDF support by about a factor of 4 in terms of overall mass transfer coefficient. Such improvement would result in significant reductions in the required membrane area to capture CO2 by a gas-liquid membrane contactor.

Poly(ionic liquid) (PIL)‐based porous membranes are extensively investigated as soft polymer actuators. While PILs have shown significant advancements in membrane fabrication and stabilization of metal nanoparticles (MNPs), research on integrating MNPs into porous membranes to achieve actuation behavior under multiple stimuli is limited. Herein, this work presents a new paradigm for designing a porous PIL‐polyacrylic acid (PAA) membrane with a distinct MNP gradient via a top‐bottom diffusion approach involving a metal salt precursor solution and NaBH4 as a reducing agent. The strong binding sites provided by PILs, combined with the gradient distribution of ‐COO− groups across the membrane cross‐section, play a significant role in controlling the MNPs' gradient distribution. Interestingly, the MNPs within the membrane display excellent catalytic activity in exothermic reactions such as H2O2 decomposition, dissipating uneven heat that quickly permeates the membrane network. This induces asymmetrical swelling of polymer chains, resulting in rapid membrane bending. Furthermore, such MNP‐loaded membrane could serve as a portable test paper for visually monitoring H2O2. This advancement paves the way for the development of intricate smart actuation materials and expands their practical applications in various real‐life scenarios. [ABSTRACT FROM AUTHOR]

Electrochromic technology that enables modulation of a material's optical properties by application of an applied voltage is utilized in smart windows. However, avoiding water absorption by lithium salt in the electrolyte necessitates complex encapsulated device assemblies that must be constructed under strict atmosphere conditions and are largely unrepairable. Herein, a lithium‐salt‐free, hydrophobic, solid‐state poly(ionic liquid) electrolyte based on strong C─F bonds that exhibits low polarizability, low moisture absorption, and a wide electrochemical window, allowing the fabrication of unencapsulated electrochromic devices with outstanding long‐term cycling and environmental stability are presented. Intimate contact between the electrolyte and the electrode is achieved through integrated in situ polymerization, providing an interface with multiple molecular interactions that impart robust adhesion, efficient ion transport, and excellent stability. To demonstrate the potential of this electrolyte for cost‐effective electrochromic smart windows, low‐cost (≈110 USD m−2), unencapsulated, removable, electrochromic "window tint film" with customizable dimensions and shapes are fabricated. [ABSTRACT FROM AUTHOR]

Abstract The escalating spread of drug‐resistant bacteria and viruses is a grave concern for global health. Nucleic acids dominate the drug‐resistance and transmission of pathogenic microbes. Here, imidazolium‐type poly(ionic liquid)/porphyrin (PIL‐P) based electrospun nanofibrous membrane and its cerium (IV) ion complex (PIL‐P‐Ce) are developed. The obtained PIL‐P‐Ce membrane exhibits high and stable efficiency in eradicating various microorganisms (bacteria, fungi, and viruses) and decomposing microbial antibiotic resistance genes and viral nucleic acids under light. The nuclease‐mimetic and photocatalytic mechanisms of the PIL‐P‐Ce are elucidated. Co‐infection wound models in mice with methicillin‐resistant S. aureus and hepatitis B virus demonstrate that PIL‐P‐Ce integrate the triple effects of cationic polymer, photocatalysis, and nuclease‐mimetic activities. As revealed by proteomic analysis, PIL‐P‐Ce shows minimal phototoxicity to normal tissues. Hence, PIL‐P‐Ce has potential as a “green” wound dressing to curb the spread of drug‐resistant bacteria and viruses in clinical settings.

[Display omitted] Poly(ionic liquid)s (PILs) bearing high ionic densities are promising candidates for carbon dioxide (CO 2) fixation. However, efficient and metal-free methods for boosting the catalytic efficiencies of PILs are still challenging. In this study, a novel family of poly(ionic liquid)-coated carbon nanotube nanoarchitectures (CNTs@PIL) were facilely prepared via a noncovalent and in-situ polymerization method. The effects of different carbon nanotubes (CNTs) and PILs on the structure, properties, and catalytic performance of the composite catalysts were systematically investigated. Characterizations and experimental results showed that hybridization of PIL with hydroxyl- or carboxyl-functionalized CNTs (CNT-OH, CNT-COOH) endows the composite catalyst with increased porosity, CO 2 capture capacity, swelling ability and diffusion rate with respect to individual PIL, and allows the CNTs@PIL to provide H-bond donors for the synergistic activation of epoxides at the interfacial layer. Benefiting from these merits, the optimal composite catalyst (CNT-OH@PIL) delivered a super catalytic efficiency in the cycloaddition of CO 2 to propylene oxide, which was over 4.5 times that of control PIL under metal- and co-catalyst free conditions. Additionally, CNT-OH@PIL showed high carbon dioxide/nitrogen (CO 2 /N 2) adsorptive selectivity and could smoothly catalyze the cycloaddition reaction with a simulated flue gas (15% CO 2 and 85% N 2). Furthermore, the CNT-OH@PIL exhibited broad substrate tolerance and could be readily recycled and efficiently reused at least 12 times. Hybridization of PIL with functionalized CNTs provides a feasible approach for boosting the catalytic performance of PIL-based solid catalysts for CO 2 fixation. [ABSTRACT FROM AUTHOR]

Hydrogen (H)‐bonding‐integration of multiple ingredients into supramolecular polyelectrolyte nanoporous membranes in water, thereby achieving tailor‐made porous architectures, properties, and functionalities, remains one of the foremost challenges in materials chemistry due to the significantly opposing action of water molecules against H‐bonding. Herein, a strategy is described that allows direct fusing of the functional attributes of small additives into water‐involved hydrogen bonding assembled supramolecular poly(ionic liquid) (PIL) nanoporous membranes (SPILMs) under ambient conditions. It discloses that the pore size distributions and mechanical properties of SPILMs are rationally controlled by tuning the H‐bonding interactions between small additives and homo‐PIL. It demonstrates that, benefiting from the synergy of multiple noncovalent interactions, small dye additives/homo‐PIL solutions can be utilized as versatile inks for yielding colorful light emitting films with robust underwater adhesion strength, excellent stretchability, and flexibility on diverse substrates, including both hydrophilic and hydrophobic surfaces. This system provides a general platform for integrating the functional attributes of a diverse variety of additives into SPILMs to create multifunctional and programmable materials in water. [ABSTRACT FROM AUTHOR]

The rational one-step design of poly(ionic liquid) solid polymer electrolyte (PIL-SPE) with outstanding ionic conductivity and inferior interfacial resistance with Li-electrode to preclude the Li-dendrite growth and interfacial instability of solid-state lithium metal batteries (ASLMBs) remains a grand challenge. Herein, we provide a s facile, one-step, and productive approach for the synthesis of PIL-SPE via the in situ polymerization of 1-vinyl-3-butylimidazolium bis(trifluoromethanesulfony)imide ([VBIm][TFSI]) in the presence of bis(trifluoromethane) sulfonamide lithium salt (LiTFSI) using azodiisobutyronitrile (AIBN) as initiator. This approach endows a compact and compatible interface between Li-electrode and PIL-SPE with an excellent ionic conductivity that depends on the Li-salt concentration. Thereby, in situ polymerization of monomer with 40 wt% LiTFSI (PIL-SPE-LiTFSI-40) revealed the highest ionic conductivity of 1.35 × 10-3 S cm−1 at 303 K and 6.16 × 10-3 S cm−1 at 353 K, besides excellent lithium transference number (0.54), oxidative stability up to 5.3 V, and constant current plating/stripping cycles for 1000 h at 0.15 mA cm−2. Meanwhile, ASLMBs composed of PIL-SPE with LiFePO4 and LiNi0.8Co0.1Mn0.1O2 cathodes delivered discharge capacities of 164.3 mA h g−1 and 155.3 mA h g−1 at 0.1 C, respectively, along with 92 % capacity retention after 100 cycles. This study may revolutionize the synthesis of PIL-SPE electrolytes for the next generation of efficient and durable ASLMBs.

The ever-growing demand for next-generation high-energy-density devices drives the development of lithium metal batteries with enough safety and high performance, in which quasi-solid-state composite electrolytes (QSCEs) with high ionic conductivity and lithium ion transference number (tLi+) are highly desirable. Herein, we successfully synthesize a kind of two-dimensional (2D) molecular brush (GO-g-PFIL) via grafting poly(ionic liquid) side-chain (poly(3-(3,3,4,4,4-pentafluorobutyl)-1-vinyl-1H-imidazol-3-ium bis(trifluoromethanesulfonyl)imide), denoted as PFIL) on the surface of 2D graphene oxide (GO) sheet. GO-g-PFIL is used as multi-functional filler to prepare novel composite membranes and corresponding QSCEs (e.g., QSCE-PH/GPFIL3/P). The as-obtained QSCE-PH/GPFIL3/P integrates features of PFIL side-chain-enhanced lithium ion conduction, poly(vinylidene fluoride-co-hexafluoropropene) backbone-induced flexibility, and GO-strengthened mechanical property. As a result, our ultrathin (21 µm) self-supporting QSCE-PH/GPFIL3/P exhibits high ionic conductivity (3.24 x 10-4 S• cm-1) and excellent tLi+ (0.82) at room temperature, and Li/LFP full cell with QSCE-PH/GPFIL3/P shows superior rate performance (high specific capacities of 79 mAh• g-1 at 30 °C and 5 C) and excellent cycling performance (high capacity retention of 91% after 500 cycles at 80 °C and 1 C). [ABSTRACT FROM AUTHOR]

With the rapid development of energy storage technology, the operation of portable and wearable devices is inseparable from high energy density power supplies. However, the demand for high performance supercapacitors in movable smart electronics is still restrained by their insufficient areal capacitance and limited power/energy densities. In addition, some electroactive materials, including metal oxides, conductive polymers, graphene, porous carbons, etc., are inevitable to use extra adhesives for the preparation of electrode materials. In this work, integrated hierarchical graphitic porous carbon membranes used as the electrodes without adhesives are successfully synthesized, via pyrolyzing poly(ionic liquid)s (PILs)‐metal organic frameworks (MOFs) composite membranes. The asymmetric supercapacitor is assembled by the carbonized PIL‐MOF composite membrane and PILs‐derived porous carbon membrane, and exhibits significant areal capacitance with remarkable power and energy densities. In the two‐electrode system, the areal capacitance can reach 9.5 F cm−2 with an energy density of 1.91 mWh cm−2. In the fabricated all‐solid‐state supercapacitors, the areal capacitance and energy density achieved 3.2 F cm−2 and 0.65 mWh cm−2, respectively, exceeding most reported ones. Therefore, the integrated carbon membrane electrodes with high areal capacitance reveal great potential in miniaturized devices, and further show a wider application scope through regulating PILs. [ABSTRACT FROM AUTHOR]

Bioactive linear choline-based copolymers were developed as micellar carriers for drug delivery systems (DDSs). The polymethacrylates containing trimethylammonium groups with p-aminosalicylate anions (PAS-based copolymers: series 1) or chloride anions (Cl-based copolymers: series 2) differing in ionic content and chain length were selected for drug loading. The diverse structures of amphiphilic copolymers made it possible to adjust the encapsulation efficiency of a well-known antibiotic, i.e., p-aminosalicylate in the form of sodium salt (PASNa) or acid (PASA), providing single drug systems. Goniometry was applied to verify the self-assembly capacity of the copolymers using the critical micelle concentration (CMC = 0.03–0.18 mg/mL) and the hydrophilicity level quantifying the surface wettability of polymer film using the water contact angle (WCA = 30–53°). Both parameters were regulated by the copolymer composition, indicating that the increase in ionic content caused higher CMC and lower WCA, but the latter was also modified to a less hydrophilic surface by drug encapsulation. The drug content (DC) in the PAS-based polymers was increased twice by encapsulation of PASNa and PASA (47–96% and 86–104%), whereas in the chloride-based polymer systems, the drug was loaded in 43–96% and 73–100%, respectively. Efficient drug release was detected for PASNa (80–100% series 1; 50–100% series 2) and PASA as complete in both series. The strategy of loading extra drug by encapsulation, which enhances the drug content in the copolymers containing anions of the same pharmaceutics, provided promising characteristics, which highlight the potential of PAS-loaded micellar copolymers for drug delivery. [ABSTRACT FROM AUTHOR]

Synergistic effects in bimetallic catalysts produce a catalyst with superior activity than a monometallic component. In this work, a novel magnetic crosslinked copoly(ionic liquid) nanohydrogel was synthesized and employed for the stabilization of AuCo bimetallic nanoparticles (Fe3O4@PolyIL‐AuCo). This material was characterized using different instrumental techniques such as FT‐IR, TGA, XPS, VSM, solid‐state UV–Vis, SEM mapping, and TEM. Results indicated a narrow size distribution of nanoparticles and high water dispersibility of Fe3O4@PolyIL‐AuCo. Using this catalyst, a series of nitroarenes were reduced to the corresponding amines in aqueous media. In addition, organic dyes were efficiently degraded by this catalyst. Different experiments dealing with the same transformation confirmed that Fe3O4@PolyIL‐AuCo exhibited higher catalytic activity than the similar monometallic Au and Co catalysts. This catalyst was recycled for at least 11 consecutive runs with very small deactivation, and TEM, VSM, and XPS confirmed the stability of the reused catalyst. [ABSTRACT FROM AUTHOR]

Despite the outstanding proton conductivity of phosphoric acid (PA)-doped polybenzimidazole (PBI) membranes as high-temperature proton exchange membranes (HT-PEMs), chemical stability is a critical issue for the operation life of PEM fuel cells (PEMFCs). Herein, we introduced polymerized [HVIM]H2PO4 ionic liquids (PIL) into an OPBI membrane to accelerate proton transfer and enhance the chemical stability of the membrane. Based on the regulation of the intrinsic viscosity of PIL, the entanglement between PIL chains and OPBI chains is enhanced to prevent the loss of PIL and the oxidative degradation of membrane materials. The PIL/OPBI membrane with the intrinsic viscosity of 2.34 dL·g−1 (2.34-PIL/OPBI) exhibited the highest proton conductivity of 113.9 mS·cm−1 at 180 °C, which is 3.5 times that of the original OPBI membrane. The 2.34-PIL/OPBI membrane exhibited the highest remaining weight of 92.1% under harsh conditions (3 wt% H2O2; 4 ppm Fe2+ at 80 °C) for 96 h, and a much lower attenuation amplitude than the OPBI did in mechanical strength and proton conductivity performance. Our present work demonstrates a simple and effective method for blending PIL with OPBI to enhance the chemical durability of the PA-PBI membranes as HT-PEMs. [ABSTRACT FROM AUTHOR]

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Metal–metal battery bears great potential for next‐generation large‐scale energy storage system because of its simple manufacture process and low production cost. However, the cross‐over of metal cations from the cathode to the anode causes a loss in capacity and influences battery stability. Herein, a coating of poly (ionic liquid) (PIL) with poly(diallyldimethylammonium bis(trifluoromethanesulfonyl)imide) (PDADMA+TFSI−) on a commercial polypropylene (PP) separator serves as an anion exchange membrane for a 3.3 V copper–lithium battery. The PIL has a positively charged polymer backbone that can block the migration of copper ions, thus improving Coulombic efficiency, long‐term cycling stability and inhibiting self‐discharge of the battery. It can also facilitate the conduction of anions through the membrane and reduce polarization, especially for fast charging/discharging. Bruce‐Vincent method gives the transport number in the electrolyte to be 0.25 and 0.04 for PP separator without and with PIL coating, respectively. This suggests that the PIL layer reduces the contribution of the internal current due to cation transport. The use of PIL as a coating layer for commercial PP separator is a cost‐effective way to improve overall electrochemical performance of copper–lithium batteries. Compared to PP and polyacrylic acid(PAA)/PP separators, the PIL/PP membrane raises the Coulombic efficiency to 99% and decreases the average discharge voltage drop to about 0.09 V when the current density is increased from 0.1 to 1 mA cm−2. [ABSTRACT FROM AUTHOR]

A new method for the preparation of polyaniline (PANI) films that have a 2D structure and can record high active mass loading (up to 30 mg cm−2) via acid-assisted polymerization in the presence of concentrated formic acid was developed. This new approach represents a simple reaction pathway that proceeds quickly at room temperature in quantitative isolated yield with the absence of any byproducts and leads to the formation of a stable suspension that can be stored for a prolonged time without sedimentation. The observed stability was explained by two factors: (a) the small size of the obtained rod-like particles (50 nm) and (b) the change of the surface of colloidal PANI particles to a positively charged form by protonation with concentrated formic acid. The films cast from the concentrated suspension were composed of amorphous PANI chains assembled into 2D structures with nanofibrillar morphology. Such PANI films demonstrated fast and efficient diffusion of the ions in liquid electrolyte and showed a pair of revisable oxidation and reduction peaks in cyclic voltammetry. Furthermore, owing to the high mass loading, specific morphology, and porosity, the synthesized polyaniline film was impregnated by a single-ion conducting polyelectrolyte-poly(LiMn-r-PEGMm) and characterized as a novel lightweight all-polymeric cathode material for solid-state Li batteries by cyclic voltammetry and electrochemical impedance spectroscopy techniques. [ABSTRACT FROM AUTHOR]

Amphiphilic double poly(imidazole ionic liquid) grafted silica (SMIL-n) was prepared by radiation grafting of hydrophilic 1-vinyl-3-ethylimidazolium bromide and hydrophobic 1-vinyl-3-octylimidazolium bromide at different ratio onto silica. The adsorption behavior of SMIL-n was investigated. The adsorption equilibrium could reach less than 45 min, and their adsorption capacity were 152–171 mg/g obtained from Langmuir model. The selectivity of SMIL-n to ReO4− increased with the increasing content of hydrophobic ionic liquid. SMIL-n displayed good reusability, excellent acid resistance and irradiation resistance. Particularly, SMIL-n showed promising for ReO4− uptake from simulated contaminated Beishan groundwater and radioactive wastewater. [ABSTRACT FROM AUTHOR]

Amphiphilic double poly(imidazole ionic liquid) grafted silica (SMIL-n) was prepared by radiation grafting of hydrophilic 1-vinyl-3-ethylimidazolium bromide and hydrophobic 1-vinyl-3-octylimidazolium bromide at different ratio onto silica. The adsorption behavior of SMIL-n was investigated. The adsorption equilibrium could reach less than 45 min, and their adsorption capacity were 152–171 mg/g obtained from Langmuir model. The selectivity of SMIL-n to ReO4− increased with the increasing content of hydrophobic ionic liquid. SMIL-n displayed good reusability, excellent acid resistance and irradiation resistance. Particularly, SMIL-n showed promising for ReO4− uptake from simulated contaminated Beishan groundwater and radioactive wastewater. [ABSTRACT FROM AUTHOR]

Herein, we report an exciting synthetic procedure for the scalable and controllable fabrication of covalently crosslinked poly(ionic liquid) (PIL) nanoporous membranes (CPILMs) in water solution under ambient conditions. We found that the pore sizes, flexibility and compositions of freestanding CPILMs can be finely tailored by a rational structural choice of PIL, diketone and aldehyde. Studies on the CPILM formation mechanism revealed that hydrogen bonding‐induced phase separation of amino‐functionalized homo‐PIL between its polar and apolar domains coupled with structural rearrangements due to the Debus Radsizewski reaction‐triggered ambient covalent crosslinking process created a stable three‐dimensionally interconnected pore system in water solution. Employing structurally stable CPILMs in ion sieving devices resulted in an excellent Li+/Mg2+ separation efficiency due to the positively charged nature and "Donann" effects. This green, facile yet versatile approach to the production of CPILMs is a conceptually distinct and commercially interesting strategy for making useful nanoporous functional polyelectrolyte membranes. [ABSTRACT FROM AUTHOR]

This study casts new aspects on using nanostructured PILs as new electrocatalyst supports in CO 2 conversion to C 1 products. [Display omitted] Herein, we report a straightforward, scalable synthetic route towards poly(ionic liquid) (PIL) homopolymer nanovesicles (NVs) with a tunable particle size of 50 to 120 nm and a shell thickness of 15 to 60 nm via one-step free radical polymerization induced self-assembly. By increasing monomer concentration for polymerization, their nanoscopic morphology can evolve from hollow NVs to dense spheres, and finally to directional worms, in which a multilamellar packing of PIL chains occurred in all samples. The transformation mechanism of NVs' internal morphology is studied in detail by coarse-grained simulations, revealing a correlation between the PIL chain length and the shell thickness of NVs. To explore their potential applications, PIL NVs with varied shell thickness are in situ functionalized with ultra-small (1 ∼ 3 nm in size) copper nanoparticles (CuNPs) and employed as electrocatalysts for CO 2 electroreduction. The composite electrocatalysts exhibit a 2.5-fold enhancement in selectivity towards C 1 products (e.g. , CH 4), compared to the pristine CuNPs. This enhancement is attributed to the strong electronic interactions between the CuNPs and the surface functionalities of PIL NVs. This study casts new aspects on using nanostructured PILs as new electrocatalyst supports in CO 2 conversion to C 1 products. [ABSTRACT FROM AUTHOR]

Drugs of abuse has drawn intense attention due to increasing concerns to public health and safety. The construction of a sensing platform with the capability to identify them remains a big challenge because of the limitations of synthetic complexity, sensing scope and receptor extendibility. Here a kind of poly(ionic liquid) (PIL) photonic crystal spheres doped with aggregation‐induced emission (AIE) luminogens was developed. As diverse noncovalent interactions involve in PIL moieties, the single sphere shows different binding affinity to a broad range of psychoactive substances. Furthermore, the dual‐channel signals arising from photonic crystal structures and sensitive AIE‐luminogens provide high‐dimensional information for discriminative detection of targets, even for molecules with slight structural differences. More importantly, such single sphere sensing platform could be flexibly customized through ion‐exchange, showing great extendibility to fabricate high‐efficiency/high‐throughput sensing arrays without tedious synthesis. [ABSTRACT FROM AUTHOR]

Ion transport in composite electrodes plays a key role in the electrochemical performance of lithium‐metal batteries (LMBs), particularly at high current densities, and hence, some works have suggested the use of ionic conducting polymers as binders. Herein, in order to assess the importance of the type of ion conduction in binders, two poly(ionic liquid) polymers were analyzed as binders in LiFePO4 (LFP) cathodes: poly(lithium 1‐[3‐(methacryloyloxy)propylsulfonyl]‐1‐(trifluoromethane sulfonyl) imide) (PMTFSI−Li), and poly(diallyldimethylammonium bis(trifluoromethane sulfonyl)imide) (PDADMA−TFSI). Their functionalities allow modulating the individual transport of their counter‐ions, Li+ and TFSI−, respectively; in comparison with conventional PVDF binder. Thus, LFP−C‐Binder cathodes, namely C−PVDF, C−PDADMA−TFSI and C−PMTFSI−Li, were evaluated in LMBs. C−PMTFSI−Li exhibited the best performance reaching the theoretical specific capacity (170.3±0.8 mAh g−1) at C/10, an outstanding capacity at 10 C (100.6±0.5 mAh g−1), and long lifespan (>500 cycles at 1 C). C−PDADMA−TFSI showed good long‐term cycling and high performance at high C‐rate, while C−PVDF ended up fading before reaching 500 cycles. Surprisingly, it was observed that the presence of ionic binders into the cathode formulation influenced on Li0 metal deposition morphology, leading to a more homogeneous plating (specially PMTFSI−Li) in comparison with PVDF; and therefore, exhibiting a mitigation of mossy lithium growth. [ABSTRACT FROM AUTHOR]

In this study, nitrogen and sulfur-codoped porous carbon material (ZC) was prepared via carbonization of the complex of hydrophobic poly(ionic liquid) (PIL) and zein through electrostatic interaction. The structure and morphology of ZCs were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM), and Raman spectroscopy. In addition, nitrogen adsorption–desorption analysis showed that ZCs were mainly mesoporous, and the pore size was in a narrow dispersity. The surface area of ZC-10 could be as high as 764 m2 g−1, and the total pore volume was 0.41 cm3 g−1. Remarkably, the specific capacitance of the electrode prepared by ZC-10 was 338 F g−1 in 2.0 M KOH at a current density of 0.1 A g−1 and presented excellent cycle stability. After 5000 cycles, the specific capacitance still remained stable. Therefore, our finding suggested a facile strategy for the fabrication of porous carbon materials with high capacitance performance through PIL and biomacromolecule composites. Considering their easy preparation and biomass source, ZCs are of great potential in the future applications of electronic devices and systems. [ABSTRACT FROM AUTHOR]

Topological geometry of poly(ionic liquid)s (PILs), such as brush‐like, knot‐like, hyperbranched and randomly coiled, often exerts a strong influence on their self‐assembly behaviors. As a primary topological form, the cyclic topology‐derived effects have not been investigated on PILs, which concerns synergy of charges and zero chain end. Herein, linear and cyclic poly(ionic liquid) copolymers (co‐PILs) with randomly distributed counter anions of B(Ph)4− and Br− by a template method in combination with a follow‐up partial anion exchange is prepared. The self‐assembly phenomena of linear and cyclic co‐PILs are studied in selective solvents, where the hydrophobic counter anions B(Ph)4− and hydrophilic counter anions Br− aggregated to form cores and corona in the assembled nanospheres, showing the average size of cyclic co‐PILs nanospheres is 46.2% smaller (≈120 nm) than linear co‐PILs nano‐assemblies (≈176 nm). Based on the CGMD simulations, the authors speculate that the spherical aggregates are formed by transitioning from micelles with gradient block‐like structures, which formed by enriched hydrophobic counter anions in the core and enriched hydrophilic counter anions in the corona. These results indicate a novel synergy of topology effects and dynamic anion movements, as revealed by cyclic co‐PIL self‐assembly in this work. [ABSTRACT FROM AUTHOR]

Thermally induced reversible up/down migration of poly(ionic liquid)s (PILs) in aqueous two‐phase systems (ATPSs) was achieved for the first time in this study. Novel ATPSs were fabricated using azobenzene (Azo)‐ and benzyl (Bn)‐modified PILs, and their upper and lower phases could be easily tuned using the grafting degree (GD) of the Azo and Bn groups. Bn‐PIL with higher GDBn could go up into the upper phase and Azo‐PIL come down to the lower phase when the temperature increased (>65 °C); this behavior was reversed at lower temperatures. Moreover, a reversible two‐phase/single‐phase transition was realized under UV irradiation. Experimental and simulation results revealed that the difference in the hydration capacity between Bn‐PIL and Azo‐PIL accounted for their unique phase‐separation behavior. A versatile platform for fabricating ATPSs with tunable stimuli‐responsive behavior can be realized based on our findings, which can broaden their applications in the fields of smart separation systems and functional material development. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Polyelectrolyte porous membranes (PPMs) belong to the most interesting classes of materials, because the synergy of tunable pore sizes and charge nature of polyelectrolyte endow them with wide‐ranging practical applications. However, owing to the water solubility and ionic nature of the polyelectrolytes, traditional polyelectrolytes are difficult to use in scalable preparation of high‐quality PPMs through the well‐developed industrial methods. Poly(ionic liquid)s (PIL) are a subclass of functional polyelectrolytes bearing ionic liquid groups in their repeating unites, inheriting the advantages of ionic liquids (ILs) and macromolecular architecture features. In recent years, along with rapid development of PIL materials chemistry, considerable and significant developments involving the novel preparation methods, and structure‐property‐function relationships of PPMs have been made. In this review, we highlight the latest discovery and proceedings of PPMs, particularly the advancements in how to tailor structures and properties of PPMs by rational structure design of PILs. The formation mechanisms of various PPMs were also discussed in detail from the viewpoint of PILs molecular structures. A future perspective of the challenges and promising potential of PPMs is cast on the basis of these achievements. We expect that these analyses and deductions will be useful for the design of useful PPMs and serve as a source of inspiration for the design of future multifunctional PPMs. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Polyelectrolyte porous membranes (PPMs) belong to the most interesting classes of materials, because the synergy of tunable pore sizes and charge nature of polyelectrolyte endow them with wide‐ranging practical applications. However, owing to the water solubility and ionic nature of the polyelectrolytes, traditional polyelectrolytes are difficult to use in scalable preparation of high‐quality PPMs through the well‐developed industrial methods. Poly(ionic liquid)s (PIL) are a subclass of functional polyelectrolytes bearing ionic liquid groups in their repeating unites, inheriting the advantages of ionic liquids (ILs) and macromolecular architecture features. In recent years, along with rapid development of PIL materials chemistry, considerable and significant developments involving the novel preparation methods, and structure‐property‐function relationships of PPMs have been made. In this review, we highlight the latest discovery and proceedings of PPMs, particularly the advancements in how to tailor structures and properties of PPMs by rational structure design of PILs. The formation mechanisms of various PPMs were also discussed in detail from the viewpoint of PILs molecular structures. A future perspective of the challenges and promising potential of PPMs is cast on the basis of these achievements. We expect that these analyses and deductions will be useful for the design of useful PPMs and serve as a source of inspiration for the design of future multifunctional PPMs. [ABSTRACT FROM AUTHOR]

Crystallinity and flame retardancy are two key properties for poly(lactic acid)(PLA) in applications. In this paper, a quaternary phosphonium salt poly(ionic liquid) (PIL) and a phosphamide (POFA) were prepared. The PIL, POFA and their blend were used to regulate the flame retardancy and crystallization behaviors of PLA using the limiting oxygen index, UL-94 vertical burning, and thermogravimetric analysis, and differential scanning calorimetry etc. The results showed that a synergistic effect exists between PIL and POFA on flame retardancy. When 6 wt% PIL/POFA (2/1) was added into PLA, its LOI value is 28.0 vol%, and achieves the UL-94 V-0 rating while the PLA composites containing 6 wt% PIL or POFA just achieve the UL-94 V2. The PIL/POFA improves the flame retardancy of PLA by melting-away mode. In addition, the crystallization rate of PLA containing PIL/POFA is faster than that of PLA/PIL and PLA/POFA. The degradation of PLA induced by PIL/POFA produces some small molecular oligomers, which enhances the molecular chain mobility and rearrangement, thus contributes to better flame retardancy and faster crystallization. • PIL and POFA were used to regulate the flame retardancy and crystallization of PLA. • PLA containing 5 wt% PIL/POFA achieves the UL-94 V0. • PIL/POFA improves the flame retardancy of PLA by melting-away mode. • Oligomers induced by PIL/POFA contribute to faster crystallization of PLA. [ABSTRACT FROM AUTHOR]

The efficient conversion of atmospheric CO 2 into high value-added chemicals remains a persistent challenge. In this study, a novel strategy for the fabrication of triazine- and amino-functionalized poly(ionic liquid)s (PILs) was reported. By virtue of the rich nitrogen species, the newly-developed PILs possessed great potential in CO 2 conversion to produce high-value chemicals. The systematic investigation illustrated that rich-nitrogen PILs could promote the cycloaddition reaction of CO 2 and epoxides through the intramolecular synergy of multiple active sites. Excellent conversion and selectivity were achieved under the mild conditions without any co-catalysts and solvents. In addition, PIL heterogeneous catalysts could be easily recovered and reused at least several times without obvious loss in activity. The density functional theory calculation demonstrated that the superior catalytic activity of rich nitrogen PILs was attributed to the synergistic effect of hydrogen bond donor and triazine ring in the catalytic process. Our finding thus presents a versatile platform for fabricating multi-functional heterogeneous catalysts for efficient CO 2 conversion. [ABSTRACT FROM AUTHOR]

• Novel ATPSs were fabricated using Azo- and Bn-functionalized PILs. • The grafting degrees of Azo and Bn had significant effects on the phase separation of ATPS. • The upper/lower phases of ATPSs with CB[8] could be inverted by photo and thermo stimuli. • The phase separation of ATPSs was regulated by host–guest interaction for the first time. Smart aqueous two-phase systems (ATPS) have aroused tremendous interests in view of their tunable phase behaviors under various stimuli, and found many potential applications in the domain of separation. Herein, poly(ionic liquid)s (PILs), functionalized by benzyl (Bn) and azophenyl (Azo) groups, were prepared through a post-synthesis modification strategy. The as-fabricated ATPSs composing of Azo-PIL and Bn-PIL exhibited a photo- and thermo-responsive two-phase to one-phase transition. However, when the host molecule cucurbituril[8] urea (CB[8]) was introduced, the as-developed PIL-based ATPSs underwent a reversible upper and lower phases inversion behaviors, which could be tuned through light irradiation or heating treatment. The study revealed that both the grafting degree (GD) of Azo/Bn groups and the feeding ratio of CB[8] played a critical role in this switchable phase inversion behavior. In addition, the sensitive hydration ability of functional PILs to external stimuli accounted for the phase inversion behavior of ATPSs. Thereby, our finding offers a novel platform for adjusting the phase separation behaviors of ATPSs via host–guest interactions. [ABSTRACT FROM AUTHOR]

Hydrogels have been widely used for fabricating flexible sensors. However, it still remains a significant challenge to construct conductive hydrogels with excellent mechanical properties. This work presents a type of double-network (DN) hydrogels composed of poly(vinyl alcohol) (PVA) and poly(ionic liquids) (PILs), which are prepared through repetitive freezing/thawing process. Taking advantage of the coordination between carboxyl groups and Fe3+ ions, the mechanical properties of the DN hydrogels are enhanced after treated with Fe3+ ions. The influence of dosage of PILs and Fe3+ ions on the mechanical properties and conductivities of DN hydrogels is investigated. The DN hydrogel P(AVIM-AA) 1 /PVA-Fe3+ 4 , which is prepared under optimal conditions, shows high tensile strength (1.75 MPa), elongation at break (375 %), and toughness (2.75 MJ m−3). P(AVIM-AA) 1 /PVA-Fe3+ 4 also displays a good conductivity of 0.65 S m−1 and a high sensing sensitivity with a gauge factor of 2.766, indicating its potential application as flexible sensors. [Display omitted] • Poly(vinyl alcohol) (PVA) and poly(ionic liquids) PILs are composted to form double-network (DN) hydrogels. • The DN hydrogels are treated with Fe3+ to further enhance mechanical properties through carboxyl-Fe3+ coordination. • The optimal sample shows good mechanical properties, conductivity, and strain sensitivity. [ABSTRACT FROM AUTHOR]

Bioactive linear choline-based copolymers were developed as micellar carriers for drug delivery systems (DDSs). The polymethacrylates containing trimethylammonium groups with p-aminosalicylate anions (PAS-based copolymers: series 1) or chloride anions (Cl-based copolymers: series 2) differing in ionic content and chain length were selected for drug loading. The diverse structures of amphiphilic copolymers made it possible to adjust the encapsulation efficiency of a well-known antibiotic, i.e., p-aminosalicylate in the form of sodium salt (PASNa) or acid (PASA), providing single drug systems. Goniometry was applied to verify the self-assembly capacity of the copolymers using the critical micelle concentration (CMC = 0.03–0.18 mg/mL) and the hydrophilicity level quantifying the surface wettability of polymer film using the water contact angle (WCA = 30–53°). Both parameters were regulated by the copolymer composition, indicating that the increase in ionic content caused higher CMC and lower WCA, but the latter was also modified to a less hydrophilic surface by drug encapsulation. The drug content (DC) in the PAS-based polymers was increased twice by encapsulation of PASNa and PASA (47–96% and 86–104%), whereas in the chloride-based polymer systems, the drug was loaded in 43–96% and 73–100%, respectively. Efficient drug release was detected for PASNa (80–100% series 1; 50–100% series 2) and PASA as complete in both series. The strategy of loading extra drug by encapsulation, which enhances the drug content in the copolymers containing anions of the same pharmaceutics, provided promising characteristics, which highlight the potential of PAS-loaded micellar copolymers for drug delivery.

Using N-vinylimidazole as the reactant and introducing different ether-based side chains pH/salt dual-sensitive poly(imidazole ionic liquid) gel (P[CnOC2vim]Cl, n=1, 2, 3) was designed and synthesized. The structure characteristic of the gel was determined by IR spectra and SEM. The swelling ratio of gel under different conditions was investigated, including releasing property for ciprofloxacin (CIP) and berberine (Ber). The results showed that P[CnOC2vim]Cl(n=1, 2, 3) gel exhibits typical pH-sensitivity and salt-sensitivity. Its swelling ratio increased first and then decreased, and reached the maximum when the value of pH was 7.4; the swelling rate is smaller under the higher concentration of the NaCl. Furthermore, P[COC2vim]Cl gel with the short ether chain has the highest release rate of CIP and Ber at pH=7.4, the release behavior is in accord with the first-order kinetic equation. With the increase of the side chain of ether group, the cumulative release rate of P[CnOC2vim]Cl(n=2, 3) gel to CIP and Ber decreased obviously, and the behavior comforts to Higuchi kinetic equation. The results suggest that P[CnOC2vim]Cl(n=1, 2, 3) gel is the pH/salt dual-sensitive potential carrier for controlled drug release.

Abstract Herein, we report a waterproof anti‐SARS‐CoV‐2 protective film prepared by spray‐coating of an aqueous colloidal dispersion of poly(ionic liquid)/copper (PIL/Cu) composite nanoparticles onto a substrate. The PIL dispersion was prepared by suspension polymerization of 3‐dodecyl‐1‐vinylimdiazolium bromide in water at 70°C. The copper acetate salt was added into the PIL nanoparticle dispersion and in situ reduced into copper nanoparticles anchoring onto the PIL nanoparticles. Despite being waterborne, the PIL in bulk is intrinsically insoluble in water and the formed coating is stable in water. The formed surface coating by PIL/copper composite nanoparticles was able to deactivate SARS‐CoV‐2 virions by 90.0% in 30 minutes and thus may effectively prevent the spread of SARS‐CoV‐2 through surface contact. This method may provide waterborne dispersions for a broad range of antivirus protective surface coatings for both outdoor and indoor applications.

Organic cathode materials have the advantages of abundant raw materials, high theoretical specific capacity, controllable structure and easy recycling. Pyrene‐4,5,9,10‐tetraone (PTO), as one of the typical organic cathode materials, achieves efficient storage and release of Na+. However, its good solubility in traditional organic liquid electrolytes is detrimental to the cyclic stability of batteries. To address this issue, the double‐layer composite gel polymer electrolyte (DLCGPE) consisting of poly (ionic liquid) gel polymer electrolyte and plastic crystal electrolyte was developed and applied to organic sodium‐metal batteries. This as‐prepared DLCGPE displays an ionic conductivity of 2.17×10−4 S cm−1 and an electrochemical window of 4.8 V. The as‐fabricated sodium‐symmetric batteries maintain interfacial stability after 500 h of cycling. Furthermore, the PTO/Na batteries could also retain a specific capacity of 201 mAh g−1 after 300 cycles, confirming that DLCGPE achieves the purpose of inhibiting PTO dissolution and maintaining batteries stability. This work broadens the application of asymmetric electrolytes in organic secondary battery. [ABSTRACT FROM AUTHOR]

The fragility and brittleness of glassy poly(ionic liquid)s (PILs) hinders the processing of ultrathin PILs membranes. This work is reported the interfacial polymerization of PILs, which enables the first preparation of defect‐free PIL nanomembranes for high flux separation of lithium (Li+, 3.8 Å) and magnesium (Mg2+, 4.3 Å) ions mixture. Aqueous solution of an amine‐functionalized PIL is brought in contact with trimesoyl chloride (TMC) hexane solution. The "amine ≈ acyl chloride" condensation reaction occurs at the "water ≈ hexane" interface to form ≈50 nm thin PILNH2‐TMC nanomembranes consisting of water‐stable nanoaggregates (≈20 nm in size). Water permeance of the PIL nanomembrane is 3 times as high as the state‐of‐the‐art polyamide nanofiltration membranes, while its MgCl2 rejection is as high as 95%. Both the structures and separation performance of PIL nanomembranes are stable versus operation time and pressure. This work opens a new avenue to process fragile PILs, such as into functional nanomembranes for ion separation. [ABSTRACT FROM AUTHOR]

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In recent years, stimuli-responsive poly(ionic liquids) (PILs) have attracted great attention. The stimuli-dependent properties, particularly the electrical properties, of multiresponsive PILs incorporating functionalized nanoparticles, however, have been less investigated. In this work, we present the synthesis, characterization, and application of PIL films incorporating pH- and thermoresponsive hybrid materials composed of gold nanoparticles functionalized with poly(2-(dimethylamino)ethyl methacrylate) (Au@PDMAEMA). The Au@PDMAEMA nanoparticles exhibit distinct responsiveness to changes in environmental pH and temperature, thereby altering the electrical properties of the PIL films blended with responsive gold nanoparticles (PIL w/Au). This research not only fills a gap in the study of electrical properties of multiresponsive nanoparticle-incorporated PILs but also extends the potential applications of PILs in various fields, including smart sensors and electronic devices.

Despite significant advancements, current self-healing materials often suffer from a compromise between mechanical robustness and functional performance, particularly in terms of conductivity and responsiveness to environmental stimuli. Addressing this issue, the research introduces a self-healable and conductive copolymer, poly(ionic liquid-co-acrylic acid) (PIL-co-PAA), synthesized through free radical polymerization, and further optimized by incorporating thermoplastic polyurethane (TPU). This combination leverages the unique properties of each component, especially ion-dipole interactions and hydrogen bonds, resulting in a material that exhibits exceptional self-healing abilities and demonstrates enhanced mechanical properties and electrical conductivity. Moreover, the PIL-co-PAA/TPU films showcase alkaline-responsive behavior, a feature that broadens their applicability in dynamic environments. Through systematic characterization, including thermogravimetric analysis, tensile testing, and electrical properties measurements, the mechanisms behind the improved performance and functionality of these films are elucidated. The conductivities and ultimate tensile strength (σ uts ) of the PIL-co-PAA/TPU films regain 80% under 8 h healing process. To extend the applications for wearable devices, the self-healing properties of commercial cotton fabrics coated with the self-healable PIL-co-PAA are also investigated, demonstrating both self-healing and electrical properties. This study advances the understanding of self-healable conductive polymers and opens new avenues for their application in wearable technology., (© 2024 The Author(s). Small published by Wiley‐VCH GmbH.)

Despite the outstanding proton conductivity of phosphoric acid (PA)-doped polybenzimidazole (PBI) membranes as high-temperature proton exchange membranes (HT-PEMs), chemical stability is a critical issue for the operation life of PEM fuel cells (PEMFCs). Herein, we introduced polymerized [HVIM]H2PO4 ionic liquids (PIL) into an OPBI membrane to accelerate proton transfer and enhance the chemical stability of the membrane. Based on the regulation of the intrinsic viscosity of PIL, the entanglement between PIL chains and OPBI chains is enhanced to prevent the loss of PIL and the oxidative degradation of membrane materials. The PIL/OPBI membrane with the intrinsic viscosity of 2.34 dL·g−1 (2.34-PIL/OPBI) exhibited the highest proton conductivity of 113.9 mS·cm−1 at 180 °C, which is 3.5 times that of the original OPBI membrane. The 2.34-PIL/OPBI membrane exhibited the highest remaining weight of 92.1% under harsh conditions (3 wt% H2O2; 4 ppm Fe2+ at 80 °C) for 96 h, and a much lower attenuation amplitude than the OPBI did in mechanical strength and proton conductivity performance. Our present work demonstrates a simple and effective method for blending PIL with OPBI to enhance the chemical durability of the PA-PBI membranes as HT-PEMs.

[Display omitted] • Hydrogen bond donor (HBD) functionalized poly(ionic liquids) were incorporated into MIL-101 framework through the encapsulation of monomers then copolymerization methods. • HBD functionalized PIL@MIL-101 exhibited excellent affinity to CO 2 , benefitted from the high BET surface area and porous structure of MIL-101 together with the incorporated poly(ionic liquid). • Due to the synergistic effects of multiple functional groups of Lewis acidic Cr sites, HBD groups and nucleophilic Br-, the HBD functionalized PIL@MIL-101 showed efficient catalytic performance for the CO 2 -epichlorohydrin cycloaddition under cocatalyst-free, solventless and mild (70 °C, 1.0 MPa, 2.5 h) reaction conditions. • HBD functionalized PIL@MIL-101 composite showed facile synthesis, easy separation, thermal and recycling stabilities for material candidate in CO 2 capture and conversion. Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH 2). The effect of different hydrogen bond donors on CO 2 -epoxide cycloaddition reaction was discussed through XPS, NH 3 -TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO 2 and epichlorohydrin, 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br-, together with the high surface area (1178 m2/g), and good CO 2 affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO 2 affinity, excellent catalytic performance in CO 2 cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO 2 capture and conversion. [ABSTRACT FROM AUTHOR]

Two‐dimensional (2D) MXene‐based lamellar membranes bearing interlayers of tunable hydrophilicity are promising for high‐performance water purification. The current challenge lies in how to engineer the pore wall's surface properties in the subnano‐confinement environment while ensuring its high selectivity. Herein, poly(ionic liquid)s, equipped with readily exchangeable counter anions, succeeded as a hydrophilicity modifier in addressing this issue. Lamellar membranes bearing nanochannels of tailorable hydrophilicity are constructed via assembly of poly(ionic liquid)‐armored MXene nanosheets. By shifting the interlayer galleries from being hydrophilic to more hydrophobic via simple anion exchange, the MXene membrane performs drastically better for both the permeance (by two‐fold improvement) and rejection (≈99 %). This facile method opens up a new avenue for building 2D material‐based membranes of enhancing molecular transport and sieving effect. [ABSTRACT FROM AUTHOR]