Search

Supramolecular polymer networks exhibit unique and tunable thermodynamic and dynamic properties that are attractive for a wide array of applications, such as adhesives, rheology modifiers, and compatibilizers. Coherent states (CS) field theories have emerged as a powerful approach for describing the possibly infinite reaction products that result from associating polymers. Up to this point, CS theories have focused on relatively simple polymer architectures. In this work, we develop an extension of the CS framework to study polymers with reversible bonds distributed along the polymer backbone, opening a broad array of new materials that can be studied with theoretical methods. We use this framework to discern the role of reactive site placement on sol–gel phase behavior, including the prediction of a microstructured gel phase that has not been reported for neutral polymer gels. Our results highlight the subtleties of thermodynamics in supramolecular polymers and the necessity for theories that capture them. [ABSTRACT FROM AUTHOR]

The fundamental understanding of the relationship between ion transport and segmental dynamics of polymer chains in polymer electrolytes is crucial for achieving high ionic conductivity at room temperature for technological applications in supercapacitors, batteries, etc. In this work, the ion dynamics and relaxation have been studied for gel polymer electrolytes (GPEs) containing P(VdF-HFP) as host polymer, adiponitrile as a plasticizer, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide as ionic liquid, and diphenylamine and copper iodide redox additives as fillers. The crystallization temperature of the ionic liquid and the melting temperature of the plasticizer play important roles in ion dynamics. The highest room-temperature ionic conductivity (3.3 × 10−3 S/cm) was obtained for the GPE filled with dual redox additives. The broadband ac conductivity spectra have been analyzed by using the Universal Power law model coupled with the Poisson–Nernst–Planck (PNP) model. The solid–solid phase transition of the ionic liquid affects the grain and grain boundary regions of the GPEs due to the presence of redox fillers. The temperature dependence of the dielectric spectra of the GPEs containing redox fillers confirms the phase transition at the crystallization temperature. The electric modulus and dielectric spectra have been analyzed by using the Havrilliak–Nigami, Kohlrausch–Williams–Watts, and derivative dielectric constant functions. The scaling of ac conductivity and modulus spectra confirms a common ion conduction and relaxation mechanism for the GPEs. The influence of dual redox additives is clearly observed in the values of ionic conductivity, ion diffusivity, and relaxation time. [ABSTRACT FROM AUTHOR]

In recent years, ionic microgels have garnered much attention due to their unique properties, especially their stimulus-sensitive swelling behavior. The tunable response of these soft, permeable, compressible, charged colloidal particles is increasingly attractive for applications in medicine and biotechnologies, such as controlled drug delivery, tissue engineering, and biosensing. The ability to model and predict variation of the osmotic pressure of a single microgel with respect to changes in particle properties and environmental conditions proves vital to such applications. In this work, we apply both nonlinear Poisson–Boltzmann theory and molecular dynamics simulation to ionic microgels (macroions) in the cell model to compute density profiles of microions (counterions, coions), single-microgel osmotic pressure, and equilibrium swelling ratios of spherical microgels whose fixed charge is confined to the macroion surface. The basis of our approach is an exact theorem that relates the electrostatic component of the osmotic pressure to the microion density profiles. Close agreement between theory and simulation serves as a consistency check to validate our approach. We predict that surface-charged microgels progressively deswell with increasing microgel concentration, starting well below close packing, and with increasing salt concentration, in qualitative agreement with experiments. Comparison with previous results for microgels with fixed charge uniformly distributed over their volume demonstrates that surface-charged microgels deswell more rapidly than volume-charged microgels. We conclude that swelling behavior of ionic microgels in solution is sensitive to the distribution of fixed charge within the polymer-network gel and strongly depends on bulk concentrations of both microgels and salt ions. [ABSTRACT FROM AUTHOR]

The electric double layer (EDL) has a pivotal role in screening charges on surfaces as in supercapacitor electrodes or colloidal and polymer solutions. Its structure is determined by correlations between the finite-sized ionic charge carriers of the underlying electrolyte, and, this way, these correlations affect the properties of the EDL and of applications utilizing EDLs. We study the structure of EDLs within classical density functional theory (DFT) in order to uncover whether a structural transition in the first layer of the EDL that is driven by changes in the surface potential depends on specific particle interactions or has a general footing. This transition has been found in full-atom simulations. Thus far, investigating the in-plane structure of the EDL for the primitive model (PM) using DFT has proved a challenge. We show here that the use of an appropriate functional predicts the in-plane structure of EDLs in excellent agreement with molecular dynamics simulations. This provides the playground to investigate how the structure factor within a layer parallel to a charged surface changes as a function of both the applied surface potential and its separation from the surface. We discuss pitfalls in properly defining an in-plane structure factor and fully map out the structure of the EDL within the PM for a wide range of electrostatic electrode potentials. However, we do not find any signature of a structural crossover and conclude that the previously reported effect is not fundamental but rather occurs due to the specific force field of ions used in the simulations. [ABSTRACT FROM AUTHOR]

Due to the importance of supercapacitors in electronic storage devices, improving their efficiency is one of the topics that has attracted the attention of many researchers. Choosing the proper electrolyte for supercapacitors is one of the most significant factors affecting supercapacitors' performance. In the present paper, we compare liquid electrolytes (ionic liquid electrolytes) and solid electrolytes (polymer electrolytes) by molecular dynamics simulation to summarize their pros and cons. We consider polymer electrolytes in linear and network configurations. The results show that although ionic liquid-based supercapacitors have a larger differential capacitance since they have a smaller operation voltage, the energy stored is less than polymer electrolyte-based supercapacitors. Also, our investigations indicate that polymer electrolyte-based supercapacitors have more mechanical stability. Therefore, they can be considered a very suitable alternative to liquid electrolyte-based supercapacitors since they do not have known liquid electrolyte problems and display better performance. [ABSTRACT FROM AUTHOR]

The aluminum ion battery (AIB) is a promising technology, but there is a lack of understanding of the desired nature of the batteries' electrolytes. The ionic charge carriers in these batteries are not simply Al3+ ions but the anionic AlCl4− and Al2Cl7−, which form in the electrolyte. Using computational analysis, this study illustrates the effect of mole ratios and organic solvents to improve the AIB electrolytes. To this end, molecular dynamics simulations were conducted on varying ratios forming acidic, neutral, and basic mixtures of the AlCl3 salt with 1-ethyl-3-methylimidazolium chloride (EMImCl) ionic liquid (IL) and an organic solvent electrolyte [dichloromethane (DCM) or toluene]. The data obtained from diffusion calculations indicates that the solvents could improve the transport properties. Both DCM and toluene lead to higher diffusion coefficients, and higher conductivity. Detailed calculations demonstrated solvents can effectively improve the formation of AlCl3⋯Cl (AlCl4−) and AlCl4−···AlCl4− (Al2Cl7−) especially in acidic mixtures. The densities, around 1.25 g/cm3 for electrolyte mixtures of AlCl3-EMImCl, were consistent with experiment. These results, in agreement with experimental findings, strongly suggest that DCM in acidic media with AlCl3 and EMImCl might provide a promising basis for battery development. [ABSTRACT FROM AUTHOR]

Developed specifically to address leakage and stability concerns inherent in liquid electrolytes, this study presents a significant advancement in polymer gel electrolyte (PGE) formulation by combining potassium iodide (KI), ammonium iodide (AI) salts, and polyvinylidene fluoride‐co‐hexafluoropropylene (PVDF‐co‐HFP) as a host polymer. The tape casting method was employed to deposit the standard TiO2 paste as the photoanode and platinum paste as the counter electrode. N3 dye was incorporated, and PVDF‐co‐HFP was used as the PGE between the electrodes. The conductivity of PGE was measured by using a digitized conductivity meter. The quasi solid‐state solar cell (QS‐DSSC) assembled using single salts (KI, and AI), and mixed cations PGE was examined via photocurrent–voltage characteristics, and electrochemical impedance spectroscopy. The augmented ionic conductivity directly influences the efficiency of DSSCs. Notably, incorporating a mixed salt (KI + AI) within the PGE enhances ionic conductivity compared to single‐salt‐based counterparts. The resultant DSSCs using mixed salt PGE exhibit a Voc of 600 mV, Jsc of 1.01 mA/cm2, FF of 0.6089, and an efficiency of 0.369%, outperforming those using KI or AI. This highlights the perceptible advantages of employing this innovative electrolyte composition to enhance solar cell performance. [ABSTRACT FROM AUTHOR]

This study displays the preparation and characterization of cross-linked rubbery hydrogel by applying gamma radiation as a fast and clean tool for industrial application. Rubbery Gel polymer was synthesized through radiation copolymerization between hydrophilic acrylamide (AAM) copolymerized with natural rubber latex at different monomer concentrations (80, 70, and 50% v/v) by using gamma radiation in order to prepare a cross-linked network between PAM and NRL (PAAM/NRL) with controllable hydrophilicity and good mechanical properties. The effect of AAM/NRL compositions and irradiation dose on the gel fraction, swelling isotherm and diffusional characteristics fully studied. The formed rubbery hydrogel with suitable swelling properties examined for the ability of adsorption of heavy metals from their aqueous solutions. Different parameters such as initial metal concentration, pH, temperature and adsorbent dosage are applied for the evaluation of the adsorption ability of the rubbery hydrogel for various toxic metals (Cu2+, Co2+, and Ni2+). The results of metal uptake showed that increasing temperature has an effective impact on the metal uptake for various types of metals tested as increasing temperature increases the rubber chains flexibility within the PAAM/NRL rubbery hydrogel. The desorption of adsorbed metal ions from the PAAM/NRL hydrogel was completed in a desorption mediums of HCL (2 and 0.5 M) and at temperature of 70 °C after 90 min. [ABSTRACT FROM AUTHOR]

Background Purpose Methods Results Conclusions Comprehensive quality assurance (QA) for a seamless workflow of high‐dose‐rate brachytherapy, from imaging to planning and irradiation, is uncommon, and QA of the source dwell position is performed in one‐ or two‐dimensions. Gel dosimetry using magnetic resonance imaging (MRI) is effective in verifying the three‐dimensional distribution of doses for image‐guided brachytherapy (IGBT). However, MRI scanners are not readily accessible, and MRI scanning is time‐consuming. Nevertheless, X‐ray computed tomography (XCT) is available for IGBT planning.In this study, we designed and developed an efficient method for QA for a seamless workflow of IGBT with a new commercially available XCT‐based polymer gel dosimeter.To enable direct insertion of brachytherapy applicators, the gelatinizing agent of the dosimeter was modified. A cylindrical polyvinyl chloride jar was filled with the modified gel dosimeter, which was subsequently used to determine the reproducibility of source dwell positions, detectability of source positional errors from intentionally introduced catheter length offsets, effect of looped source transfer tubes on the average displacement, extent of inter‐observer variation, and gel robustness following multiple needle‐insertions. Three ProGuide sharp needles were inserted into the jar. The dwell time at each point was determined to identify the irradiated volume with a diameter of approximately 10 mm on XCT images. All the times were the same. The plan was delivered using an afterloader with an Ir‐192 radioactive source, and the irradiated gel dosimeter was scanned using an XCT scanner. The subtracted images were generated from pre‐ and post‐irradiated images. Volumes with incremented Hounsfield units were manually identified and contoured. The centroid of the volume was defined as the measured source dwell position. Subsequently, planned source dwell positions were extracted from the DICOM file of the plan. Finally, the source dwell positions in plan and irradiated gel were compared in three axes.The hardness of the dosimeter was 1250% greater than that of the previously reported gel dosimeter. Source dwell positions were visually identified in the XCT image. Testing of CT acquisition, planning, irradiation, and analysis was completed in approximately 1 h. In the reproducibility test of source dwell positions, created by inserting three needles (each with three source dwell positions), the average displacements of the source positions from the first source dwell position were within 0.5 mm in all three directions. In the detectability test, displacements were less than 1 mm in the x–y plane but greater than 1 mm in the z‐axis, which was the source path direction. When errors of 1–3 mm were intentionally introduced, the measured displacement was within 0.7 mm of the median (range: 0.21–1.65 mm) of intentional errors. When the transfer tube was looped, the source dwell position displaced by approximately 1 mm. After 20 needle‐insertions, the source dwell position displacement was within 1 mm. The maximum inter‐observer variation of contouring was 0.57 mm.The XCT‐based gel dosimeter enabled verification of three‐dimensional source dwell positions for a seamless workflow of IGBT with high precision and efficiency. [ABSTRACT FROM AUTHOR]

Polymer gels are fascinating soft materials and have become excellent candidates for wearable electronics, biomedicine, sensors, etc. Synthetic gels usually suffer from poor mechanical properties, and integrating good mechanical properties, adhesiveness, stability, and self‐healing performances in one gel is more difficult. Herein, polymerization‐induced self‐assembly (PISA) providing PEG‐gels with an overall improvement in their comprehensive performances is reported. PISA synthesis is carried out in PEG (solvent) to efficiently produce various nanoparticles, which are used as the nanofillers in the subsequent synthesis of PEG‐gels with dynamic micelle‐crosslinked hierarchical structures. Compared to hydrogels, PEG‐gels show excellent long‐term stability due to the nonvolatile feature of PEG solvent. The hierarchical PEG‐gels (with nanofillers) exhibit better mechanical and adhesive properties than the homogeneous‐gels (without nanofillers). The energy dissipation mechanism of the PEG‐gels is analyzed via stress relaxation and cyclic mechanical tests. High‐density hydrogen bonds between the micelles and PAA matrix can be broken and reformed, endowing better self‐healing properties of the dynamic micelle‐crosslinked PEG gels. This work provides a simple strategy for producing hierarchical structural gels with enhanced properties, which offers fundamentals and inspirations for the designing of various advanced functional materials. [ABSTRACT FROM AUTHOR]

The uncontrollable lithium (Li) dendrites growth and complex electrode/electrolyte interface (EEI) problems are hindering the further application of high energy density lithium metal batteries (LMBs) in practice. Herein, a bilayer heterostructure gel polymer electrolyte (BGPE) is designed by directly curing functional boron‐containing monomers on the electrode surface to ensure excellent conductivity while solving the interface problems, achieving durable high voltage resistance and Li dendrites suppression. The unoccupied p‐orbital boron moiety of the 3D crosslinked network in BGPE not only improves the Li+ transference number (0.78), but also enhances the interfacial stability of the Li metal and inhibits the dendrites growth by anchoring PF6− anions and regulating the uniform Li deposition, thus ensuring a long cycle for Li/BGPE/Li cells. In addition, the functional additives tris(trimethylsilyl) phosphite and tris(pentafluorophenyl)borane can preferentially oxidize and decompose to form stable B, F, and Si‐rich EEIs, and effectively regulate the uniform growth of EEI. Thus, the LiNi0.5Co0.2Mn0.3O2/BGPE/Li and LiFePO4/BGPE/Li full cells exhibit stable cycling and excellent rate performance. This work provides a guiding design direction to address the EEI problems for high energy density LMBs. [ABSTRACT FROM AUTHOR]

Reaping the benefits of the burgeoning investigation of gels in recent decades, flexible electronics based on conductive gels have been extensively explored. Gels consisting of polymer networks and solvents provide ideal platforms for fabricating flexible electronics due to their soft mechanical nature, excellent biocompatibility, water‐like environment, and ease of processing. The majority of investigations of flexible electronics primarily focus on functionalities such as sensing capability, energy density, luminance, fluctuating frequency, and so on, whereas the distinguishing feature of flexible electronics lies in its inherent deformable mechanics in comparison to metal‐ or semiconductor‐based stiff electronics. However, the comprehensive design and investigation of the mechanical properties of deformable conductive gels have not received sufficient attention to improve the overall performance of flexible electronics. A comprehensive summary is provided, listing six crucial mechanical parameters—stretchability, modulus, strength, elasticity, hysteresis, and fatigue—which exert significant influence on the functionalities of flexible electronics. This review aims to direct researchers’ attention toward the mechanical design of deformable conductive gels and presents representative strategies for their mechanical modulation. [ABSTRACT FROM AUTHOR]

Gel polymer electrolytes (GPEs) hold great promise for the practical application of lithium metal batteries. However, conventional GPEs hardly resists lithium dendrites growth and maintains long‐term cycling stability of the battery due to its poor mechanical performance. Inspired by the slide‐ring structure of polyrotaxanes (PRs), herein we developed a dynamic slide‐crosslinked gel polymer electrolyte (SCGPE) with extraordinary stretchability of 970.93 % and mechanical strength of 1.15 MPa, which is helpful to buffer the volume change of electrodes and maintain mechanical integrity of the battery structure during cycling. Notably, the PRs structures can provide fast ion transport channels to obtain high ionic conductivity of 1.73×10−3 S cm−1 at 30 °C. Additionally, the strong polar groups in SCGPE restrict the free movement of anions to achieve high lithium‐ion transference number of 0.71, which is favorable to enhance Li+ transport dynamics and induce uniform Li+ deposition. Benefiting from these features, the constructed Li|SCGPE‐3|LFP cells exhibit ultra‐long and stable cycle life over 1000 cycles and high‐capacity retention (89.6 % after 1000 cycles). Even at a high rate of 16 C, the cells deliver a high capacity of 79.2 mAh g−1. The slide‐crosslinking strategy in this work provides a new perspective on the design of advanced GPEs for LMBs. [ABSTRACT FROM AUTHOR]

Compared with conventional lithium‐ion battery systems, anion‐intercalation in graphite cathodes opens avenues for the development of batteries with groundbreaking power density. This study explores the enhancement of dual‐ion batteries (DIBs) by gel polymer electrolyte (GPE) enhanced with surface‐charged nanoclays, focusing on overcoming traditional challenges such as electrolyte decomposition, anion‐solvent co‐intercalation, and interfacial instability at the graphite cathode. Three nanoclays including montmorillonite, kaolinite, and halloysite are compared by incorporating them into GPE and evaluating their effect on the electrochemical properties, ion conduction, and mechanical integrity of DIBs. Particular attention is paid to the halloysite because of its differential internal and external surface charges, which generate charge separation, facilitate optimal lithium‐ion transport, and mitigate undesirable anion‐solvent interactions. These results indicate that halloysite‐incorporated GPE (HS‐G) significantly improves DIB performance, as demonstrated by extended cycle life, robust capacity retention at fast charge/discharge rates of 20 C, and operational stability over a wide temperature range (0–60 °C). These improvements are attributed to the unique structural advantages of HS‐G, including effective charge separation, enhanced anion diffusion, and reduced solvent co‐intercalation, which provide an environmentally friendly and cost‐effective approach to advanced DIB applications. [ABSTRACT FROM AUTHOR]

This study presents a novel approach to developing eco‐friendly dye‐sensitized solar cells (DSSCs) using natural and renewable materials for gel polymer electrolytes (GPEs), reducing reliance on unsustainable solvents. Water is added to polar aprotic solvents, specifically ethylene carbonate/propylene carbonate (EC/PC), across various mass fractions (0:100 to 100:0). An amphiphilic hydroxypropyl cellulose (HPC) natural polymer is employed to formulate GPEs within this water‐EC/PC cosolvent system, achieving successful gelation up to 50:50 mass fractions. Incorporating water reduced the gel strength and viscosity of the GPEs. Water acted as a plasticizer, enhancing the polymer chains mobility, and creating a more flexible and permeable structure. This increased ion diffusion coefficients and ion mobility, resulting in a maximum ionic conductivity of 18.17 mS cm−1. The highest efficiency achieved in DSSCs using these GPEs is 5.81%, with elevated short‐circuit current density and reduced recombination losses. However, some compositions experienced syneresis, affecting their stability. The GPE with a 40:60 mass fraction exhibited superior long‐term stability because it is free from syneresis, though it achieved a lower efficiency (4.83%), making it the best‐performing sample. This work demonstrates the feasibility and benefits of using gel polymer electrolytes in an aqueous system, improving DSSC efficiency and sustainability. [ABSTRACT FROM AUTHOR]

Water‐cut control is critical to efficient reservoir development. In this investigation, a host‐guest inclusion polymer gels system with self‐assembly features was constructed stemming from the host‐guest recognition mechanism. Subsequently, the elements affecting polymer viscosity were discussed. Eventually, the injectivity and plugging performance of the host‐guest inclusion system were measured by core displacement tests. The results indicated that the optimum synthesis temperature of the host polymer and guest polymer were 30 °C and 40 °C, separately, and the optimum total monomer content should be 20 wt%. The polymer system had excellent thickening properties and shearing resistance resulting from host‐guest inclusion interaction and physical hydrophobic association. Meanwhile, it had better plugging performance than host polymer or guest polymer alone. This profile control agent system provides a novel method for settling deep profile control in oilfields. [ABSTRACT FROM AUTHOR]

Ionic electroactive polymer gels are widely employed as actuators in soft robotics due to their ability to undergo rapid mechanical deformation under low‐voltage. How to improve the performance of the ionic electroactive polymer actuators is always the focus of research in this field. Optimizing the migration of ions within the actuator is crucial for enhancing the actuation performance. In this regard, this study innovatively introduces slot‐die‐printing technology to fabricate gel actuation layers characterized by high smoothness and uniform particle distribution, achieving seamless integration between the electrodes and gel actuation layers, while mitigating issues associated with ion accumulation due to polymer clustering. Furthermore, this study attempts to add lactic acid to the traditional CS‐PVA‐IL gel, effectively strengthening the connection between CS and PVA, and promoting smooth ion transport within the gel. The results demonstrate that the actuators prepared in this study achieved a high‐bending‐strain of 0.35%, with a retention rate of 91% for actuation displacement after 10 000 cycles, showcasing superior actuation performance compared to existing research. The fabrication method proposed in this study is simple and highly reproducible, making it suitable for widespread industrial application, and providing a new approach for future industrial production of soft robotics. [ABSTRACT FROM AUTHOR]

A series of novel gel polymer electrolytes (GPEs) was developed for quasi-solid-state dye-sensitized solar cells (DSSCs), to enhance their performance via mixed counterion effect. Here, LiI, CsI, tetrahexylammonium iodide (Hex4NI), and 1-methyl-3-propylimidazolium iodide (MPII) were used as iodide salts for the preparation of this new GPE. The electrolyte series was investigated by varying the molar fractions of LiI and CsI, keeping the molar fractions of Hex4NI and MPII constant. The molar composition of the iodide salts in electrolytes is MPII0.25(Hex4NI)0.8CsI(2-x)LiIx, where x is the variable. The temperature dependence of conductivity showed Vogel-Tammann-Fulcher behavior. The sample with x = 0.72, where LiI to CsI to Hex4NI to MPII molar ratio is 72:48:80:25, which gave 8.42 mS cm−1 at 30 °C, displayed the maximum conductivity at all the temperatures. The dependence of the complex AC conductivity on frequency is examined in detail to study the impacts of dielectric polarization effects of the GPEs. Quasi-solid-state DSSCs were constructed by utilizing six-layered TiO2 photoelectrodes, Pt counter electrode, and the novel GPE series. The three-salt electrolytes, containing LiI only and CsI only, containing DSSC showed efficiencies of 5.72% and 3.53% respectively. The four-salt system, which is composed of LiI to CsI to Hex4NI to MPII with a molar ratio of 96:24:80:25, demonstrated the highest solar cell efficiency of 7.42%, due to the collective contribution of Hex4N+, MPI+, Cs+, and Li+ ions in improving the charge transport in the electrolyte system. This study shows that DSSC performance can greatly be improved by optimizing counterion ratios without changing total ions in the electrolyte. [ABSTRACT FROM AUTHOR]

The room temperature ionic conductivity of polyethylene oxide (PEO)-based polymer electrolytes is low, the electrochemical window is narrow, and the mechanical strength is relatively poor. In this work, a cross-linking gel-based solid composite polymer electrolyte (CG-SCPE) was synthesized by introducing electrochemically stable carbonate-based functional groups. The synthesized CG-SCPE presents excellent tensile strength (26 MPa) and a wide electrochemical stability window (> 4.5 V vs. Li/Li+). Meanwhile, the in situ polymerization method induced by thermal heating resulted in good compatibility between electrodes/electrolytes. In addition, the assembled LiNi0.5Co0.2Mn0.3O2/CG-SCPE/Li battery exhibited satisfactory electrochemical performance. Therefore, the gel polymer electrolyte CG-SCPE with cross-linking network provides the possibility for future application of safe and high-performance solid-state lithium metal batteries. The results indicate that the introduction of cross-linking framework can simultaneously improve the mechanical strength, thermal stability, and electrochemical performance of solid polymer electrolyte. [ABSTRACT FROM AUTHOR]

Lithium metal batteries (LMBs) are desirable candidates owing to their high‐energy advantage for next‐generation batteries. However, the practical application of LMBs continues to be constrained by thorny safety issues with the formation and growth of Li dendrites. Herein, the ZIF‐67 MOFs are in situ coupled onto a single face of 3D porous nanofiber to fabricate an asymmetric Janus membrane, harnessing their anion adsorption capabilities to promote the uniform deposition of Li ions. In addition, the poly(ethylene glycol) diacrylate and trifluoromethyl methacrylate are introduced into nanofiber skeleton to form Janus@GPE, which preferentially reacts with Li metal to form a LiF‐rich stable SEI layer to inhibit Li dendrite growth. Importantly, the synergistic effect of the MOFs and stable solid electrolyte interphase (SEI) layer results in superior cycling performance, achieving a remarkable 2500 h cycling at 1 mA cm−2 in the Li/Janus@GPE/Li configuration. In addition, the Janus@GPE electrolyte has a certain flame retardant, which can self‐extinguish within 3 s, improving the safety performance of the batteries. Consequently, the Li/Janus@GPE/LFP flexible pouch cell exhibits favorable cycling stability (the capacity retention rate of 45 cycles is 91.8% at 0.1 C). This work provides new insights and strategies to improve the safety and practical utility of LMBs. [ABSTRACT FROM AUTHOR]

Clusterization‐triggered emissive (CTE) materials have attracted great attention in recent years. The regulation of the emission property of materials with CTE property through supramolecular interactions is an excellent strategy for the construction of smart fluorescent materials. In this work, we have prepared a regulatable supramolecular polymer network with CTE properties through pillararene‐based host−guest interactions. The pillar[5]arene‐grafted poly(methyl methacrylate) (PMMA) showed a classic CTE character. After adding Brooker's merocyanine‐grafted polymer to the solution of the pillar[5]arene‐containing PMMA, the supramolecular polymer network gel formed by the host−guest interactions between pillararene and Brooker's merocyanine guest. This supramolecular network showed brighter fluorescence than the pillar[5]arene‐grafted PMMA in the solid state. In addition, the fluorescence emission of the supramolecular network can be further regulated by pH conditions. After adding an acid, the Brooker's merocyanine‐containing guest polymer was protonated, and the supramolecular network changed to a protonated network through host−guest interactions between protonated Brooker's merocyanine guest and pillararene. Interestingly, the fluorescence was quenched when the supramolecular network turned into the protonated network. After adding a base, the protonated network can convert back to the original network, along with recovery of the fluorescence. Therefore, the regulation of the fluorescence of the supramolecular polymer materials with CTE was successfully realized by pillararene‐based host−guest interactions. Furthermore, this tailorable fluorescent supramolecular polymer network system was applied as an information encryption material. [ABSTRACT FROM AUTHOR]

In comparison with solid polymer electrolytes, hydrogel polymer electrolytes are now a potentially suitable candidate for aqueous zinc‐ion batteries (ZIBs). Generally, a hydrogel is mainly composed of a hydrophilic polymer network with a high water absorption propensity and the distinctive properties of being soft and wet, becoming a gel and solid polymer electrolyte in terms of ionic conductivity and mechanical properties. All these unique characteristics of electrolytes combine with an appropriate anode and cathode materials to deliver high safety, low cost, environmental friendliness, and excellent electrochemical performance in ZIB. Nevertheless, there is no comprehensive overview on the development of hydrogel electrolytes for ZIBs available. Therefore, this study focuses on the most recent breakthroughs in hydrogel‐based polymer electrolytes for ZIBs. Further, a brief explanation of various types of hydrogel electrolytes as well as the electrochemical performance of different polymer‐based electrolytes arediscussed. Finally, the challenges of hydrogel electrolytes for currently established Zn‐ion batteries and the future research directions towards the high‐performance flexibile ZIBs are explored. [ABSTRACT FROM AUTHOR]

Noticeable progress has been made in mechanically strong and tough of polymer gels, whereas this consistency between mechanical robustness and perfect elasticity remains a challenge. Here, a simple method is conducted for fabricating hyperelastic hydrogels based on the proposed molecular engineering of dissipative energy taking advantage of two distinct interactions with great difference of binding energy. This molecular engineering of dissipative energy refers to the complementarity at the molecular level between strong and weak interactions: the strong interaction provides the mechanical strength, the weak interaction eliminates the yielding and dense chain entanglements are further implanted, resulting in the perfect hyperelasticity. Such a complementarity in reformation time and binding energy of two interactions triggers a wide range of controllable window for regulating mechanical performances, filling the current gap in the design of hyperelasticity using only high‐order structures. The resultant hyperelastic hydrogels exhibit remarkable tensile strength and linear elastic deformation, but also outstanding swelling resistance, biocompatibility, hydrophilicity, and skin‐like elastic moduli. The work thus provides a promising concept for designing elastic and robust polymer gels and brings a new perspective in the combination of mutually incompatible mechanical properties, which will likely promote innovative applications in bioengineering and bioelectronics. [ABSTRACT FROM AUTHOR]

The high‐speed impact‐resistanct materials are of great significance while their development is hindered by the intrinsic tradeoff between mechanical strength and energy dissipation capability. Herein, the new chemical system of molecular granular material (MGM) is developed for the design of impact‐resistant materials from the supramolecular complexation of sub‐nm molecular clusters (MCs) and hyper‐branched polyelectrolytes. Their hierarchical aggregation provides the origin of the decoupling of mechanical strengths and structural relaxation dynamics. The MCs' intrinsic fast dynamics afford excellent high‐speed impact‐resistance, up to 5600 s−1 impact in a typical split‐Hopkinson pressure bar test while only tiny boundary cracks can be observed even under 7200 s−1 impact. The high loadings of MCs and their hierarchical aggregates provide high‐density sacrificial bonding for the effective dissipation of the impact energy, enabling the protection of fragile devices from the direct impact of over 200 m s−1 bullet. Moreover, the MGMs can be conveniently processed into protective coatings or films with promising recyclability due to the supramolecular interaction feature. The research not only reveals the unique relaxation dynamics and mechanical properties of MGMs in comparison with polymers and colloids, but also develops new chemical systems for the fabrication of high‐speed impact‐resistant materials. [ABSTRACT FROM AUTHOR]

In the previous study (Green Chem., 2023, 25, 3418), highly stretchable and mechanically tough poly(methyl acrylate) (pMA) microparticle‐based elastomers can be formed by drying a microparticle‐containing aqueous dispersion. This discovery has the potential to overcome the mechanical weakness of industrially produced aqueous latex films. However, in 3D‐arranged particle films, structural complexity, such as the existence of defects, makes it difficult to clearly understand the relationship between the particle film structure and its mechanical properties. In this study, 2D‐ordered pMA particle monolayers at the air/water interface of a Langmuir trough are prepared. Under high compression at the air/water interface, the microparticles contact their neighboring particles, and the resulting monolayers can be successfully transferred onto a solid substrate. The compression of the monolayer films is linked to an increase in the elastic modulus of the monolayer film on the solid substrate as evident from the local Young's modulus mapping using atomic force microscopy. Thus, pMA particle films with different mechanical properties can be created using a Langmuir trough. [ABSTRACT FROM AUTHOR]

Non‐conjugated luminescent polymers have received much attention due to their excellent flexibility, processability, and biocompatibility. However, the single emission color and low solid‐state luminescence efficiency restrict their further development. Herein, by introducing carboxyl‐terminated alkyl chains on the rigid and helical polymaleimide backbone, a series of non‐conjugated luminescent polymers are designed and synthesized. Due to the "spring lock" formed by the synergism of scalable helical main chains and flexible alkyl side chains, these polymers exhibit effective cluster luminescence with thermally activated delayed fluorescence (TADF) property, thereby significantly improving the solid‐state luminescence efficiency with the quantum yield up to 59.6%. The TADF emission wavelengths of the polymer powders can be tuned from 498 to 639 nm through changing reaction solvents, because the conformation of helical chains forming clusters is sensitive to solvent polarity. Interestingly, metal ions can induce the polymers to construct self‐repairing cluster luminescence gels, which show excellent potential applications in ammonia detection and information encryption. This work not only provides an effective design strategy for the colorful cluster luminescence with high‐efficiency TADF, but also further reveals the cluster luminescence mechanism and enlightens the promising applications of cluster luminescent gels. [ABSTRACT FROM AUTHOR]

AbstractElectrochromic devices (ECDs) have broad application prospects in smart windows, low-power displays, anti-glare rearview mirrors, and so on. The electrolyte layer is one of the crucial components of ECDs acting as an interface layer between two electrodes to provide ions transport. Conventional liquid electrolytes have disadvantages of easy leakage, low safety and complex encapsulation, while inorganic solid electrolytes (ISEs) have very poor room temperature conductivity. Polymer electrolytes are composites consisting of polymeric matrices, solvents, conductive salts and curing agents, including solid polymer electrolytes (SPEs), gel polymer electrolytes (GPEs) and composite polymer electrolytes (CPEs). They are widely used in ECDs because of their excellent ionic conductivity, superior electrochemical stability, high transparency and simplicity of processing. This review provides a detailed discussion of the types, mechanisms, characteristics and preparation methods of polymer electrolytes for ECDs. The latest research progresses in the design and application of CPEs based on poly(ethylene oxide) (PEO), poly(methyl methacrylate) (PMMA), poly(vinylidene fluoride) (PVDF) and poly(vinyl alcohol) (PVA) are highlighted, and the potential applications of polymer electrolytes in the field of electrochromism are reviewed. Furthermore, the future development of polymer electrolytes in ECDs with stability, significant coloration efficiency and high ionic conductivity is discussed. [ABSTRACT FROM AUTHOR]

[Display omitted] • The multifunctional additive HCCP-TMP was innovatively synthesized by combining the free radical trapping unit—hindered amine with the high-efficiency flame retardant element—HCCP. • HCCP-TMP significantly increased the upper limit of electrochemical window of the polyacrylate gel electrolyte, improving the compatibility with the nickel-rich high-voltage cathode NCM811. • The addition of HCCP-TMP significantly improved the cycling stability and rate performance of the polyacrylate gel electrolyte at high voltages. • 1 wt% HCCP-TMP can make the polyacrylate-based gel electrolyte non-flammable, and the equipped NCM811//graphite pouch battery will not exhibit fire behavior during thermal runaway, improving the fire safety of the battery. For high energy density lithium-ion batteries (LIBs) with nickel-rich ternary cathodes, the chemical degradation of electrolytes caused by free radical reactions and the hazards of thermal runaway have always been significant challenges. Inspired by the free radical scavenging of living organisms and multiphase synergistic flame retardant mechanism, we innovatively designed and prepared a multifunctional flame retardant HCCP-TMP that combines flame retardancy and free radical scavenging by combining hindered amine and cyclophosphazene. Only 1 wt% HCCP-TMP can make the polyacrylate-based gel polymer electrolyte (GPE) incombustible. Moreover, the equipped NCM811//Graphite pouch cells don't exhibit combustion behavior after thermal runaway and can resist mechanical abuse. Based on the above noncombustible GPE, the NCM811//Li battery exhibits capacity retention rate of 82.2 % after 100 cycles at a current density of 2 C and in the voltage range of 3.0–4.7 V, exhibiting excellent cyclability under high voltage. This simple molecular design simultaneously improves the fire safety and high voltage stability, demonstrating enormous application potential in the field of advanced LIBs with high safety and high energy density. [ABSTRACT FROM AUTHOR]

Single ion conducting gel polymer electrolytes (GPEs) are characterized as having a certain amount of ionic liquid or solvent incorporated into a single ion-conducting polymer matrix and may afford the advantages of high conductivity and low electrolyte polarization under battery operation. Single ion conducting polymers often suffer from low conductivity due to their reliance on polymer segmental motion to achieve sufficient ion mobility. However, by incorporating specific solvents into a single ion conducting matrix, mobility of the polymer can be enhanced while still maintaining the advantages of single ion conduction. Although many of the solvents used to swell GPEs are mixtures of flammable organic solvents (such as dimethyl carbonate), there are many potential non-reactive, low vapor pressure solvents that could effectively solvate alkali-ion based GPEs and plasticize the polymer matrix to enhance ion conductivity. Adipate-based solvents are a group of non-volatile plasticizers with low viscosities and low vapor pressures at room temperature derived from adipic acid. The ester groups in these solvents may effectively solvate alkali ions such as Na+, leading to higher conductivity, while circumventing issues of flammability found in current alkali-ion conducting electrolytes. This study investigates the properties of sodium-ion conducting GPEs that have been swollen with varying adipate-based solvents and the subsequent dielectric response from the solvent addition. Dielectric relaxation spectroscopy was used to characterize the Na+ conductivity, static dielectric constant, ion-conducting content, and mobility of the membranes before and after the non-volatile solvent uptake. Understanding this relationship will pave the path toward safer, more efff cient solid-state polymer electrolytes for battery applications. [ABSTRACT FROM AUTHOR]

For the next generation of lithium batteries, polymer‐based electrolytes are promising candidates for resolving issues from liquid electrolytes such as leakage, flammability, and explosion. Various attempts have been carried out to develop polymer electrolytes based on poly(ethylene oxide) (PEO), polyacrylonitrile, polyvinylidene fluoride, etc., resulting in suppression for dendrite growth on Li metal and mechanical support against internal or external shock as well. Among these polymer electrolytes, PEO has been widely used due to their relatively high ionic conduction through the hopping of Li ions. Herein, poly(GAP‐co‐THF) diol (PGT) having a similar main chain to PEO while containing azide groups in a side chain is synthesized. To enhance the processability of polymer electrolytes, the thermal crosslinking process is performed via azide‐alkene cycloaddition between PGT and poly(ethylene glycol) diacrylate with lithium bis(trifluoromethanesulfonyl)imide without any initiators and organic solvents. Thickness controllable thin film of polymer electrolyte is obtained after the crosslinking process, resulting in outstanding advantages with respect to stacking of batteries. To check the electrochemical stabilities and cell performances of these polymer electrolytes, cyclic voltammetry, linear symmetric voltammetry, LiFePO4∥Li cell, and Li symmetric cell tests are accomplished. [ABSTRACT FROM AUTHOR]

In the field of energy technologies, self‐charging batteries are receiving extensive attention. However, the existing technologies are highly dependent on the available sources of O2, have long self‐charging duration, and have complex architectures. Herein, a novel ultrafast chemical self‐charging Zn‐quinhydrone polymer gel (QPG) battery, composed of acid/base free quinhydrone as a cathode material is reported. The prepared Zn–QPG battery exhibits a specific capacity of 209.7 mAh g−1 at 10C rate and maintains 86.4% of the initial discharge capacity even after 3000 cycles with a high coulombic efficiency of 99.4%. The aqueous amphiphilic block co‐polymer‐driven selective oxidation of hydroquinone (HQ) to benzoquinone (BQ) compels the chemical self‐charging feature wherein the device attains ≈1.1 V within ten minutes of complete discharge. The chemical self‐charging generated a high specific capacity of 197.8 mAh g−1 at 10C rate with a capacity retention of 91.2% after 100 cycles. Moreover, a flexible Zn–QPG battery also demonstrates excellent rechargeability and power‐delivering ability even in a wrist‐bend geometry. This work paves the way to develop ultrafast energy storage systems, which are not dependent on an external power supply and broaden the horizon of aqueous zinc–organic batteries. [ABSTRACT FROM AUTHOR]

Rechargeable Ca batteries offer the advantages of high energy density, low cost, and earth‐abundant constituents, presenting a viable alternative to lithium‐ion batteries. However, using polymer electrolytes in practical Ca batteries is not often reported, despite its potential to prevent leakage and preserve battery flexibility. Herein, a Ca(BH4)2‐based gel‐polymer electrolyte (GPE) is prepared from Ca(BH4)2 and poly(tetrahydrofuran) (pTHF) and tested its performance in Ca batteries. The electrolyte demonstrates excellent stability against Ca‐metal anodes and high ionic conductivity. The results of infrared spectroscopy and 1H and 11B NMR indicate that the terminal ─OH groups of pTHF reacted with BH4− anions to form B─H─(pTHF)3 moieties, achieving cross‐linking and solidification. Cyclic voltammetry measurements indicate the occurrence of reversible Ca plating/stripping. To improve the performance at high current densities, the GPE is supplemented with LiBH4 to achieve a lower overpotential in the Ca plating/stripping process. An all‐solid‐state Ca‐metal battery with a dual‐cation (Ca2+ and Li+) GPE, a Ca‐metal anode, and a Li4Ti5O12 cathode sustained >200 cycles, confirming their feasibility. The results pave the way for further developing lithium salt‐free Ca batteries by developing electrolyte salts with high oxidation stability and optimal electrochemical properties. [ABSTRACT FROM AUTHOR]

Superabsorbent polymer gels are widely used in commercial areas, such as in hygiene products. A key aspect in these and other applications is the gel swelling kinetics, and a key factor of influence on that is the hydrophobicity of the gel. This paper reports on the synthesis of superabsorbent polymer microgel particles with four differently hydrophobic crosslinkers: N,N'‐methylenebisacrylamide (MBAA), N,N'‐ethylenebisacrylamide (EBAA), N,N'‐propylenebisacrylamide (PBAA), and N,N'‐butylenebisacrylamide (BBAA). This work uses droplet‐based microfluidics to produce uniform and well‐defined microgel specimen and study the influence of the crosslinker hydrophobicity on the swelling kinetics. In particular, this work determines swelling constants and their dependencies on the temperature of the swelling medium as well as the activation energies of swelling in relation to the crosslinker hydrophobicity. This work finds two competing effects, leading to a narrow window in which the activation energy of the swelling of the microgels decreases with increasing crosslinker hydrophobicity. [ABSTRACT FROM AUTHOR]

Rechargeable zinc-ion batteries (ZIBs) have grown in popularity due to their low cost and the abundance of resources. However, there has been little research into the development of gel polymer electrolytes (GPEs) for high voltage and capacity ZIBs. The use of agricultural waste as a polymer electrolyte (PE) is gradually increasing in order to support a circular economy. This study focuses on the utilization of cellulose derived from coffee silverskin (CS); coffee silverskin is a by-product generated during coffee roasting. We employ a reasonable approach to create the coffee silverskin cellulose (CSC)/polyacrylamide (PAM) GPE, with the goal of achieving good properties and improved battery performance. An investigation was conducted to determine the effect of CSC content in GPEs on ZIB characteristics. The cellulose derived from CS had a crystallinity index (CrI) of 64.60%. The optimal amount of cellulose added to the acrylamide monomer (AM) for the GPE of ZIB was found to be 2.5 mg (CSC/AM/salt weight ratio of 0.01/6/23). This amount resulted in the highest electrochemical stability and a cycling time of approximately 226 h. Furthermore, the PAM/Cellulose 2.5-based GPE exhibited increased Young's modulus and tensile strength compared to the pure PAM. The electrochemical impedance spectroscopy (EIS) test revealed a diffusion resistance of 27.47 Ω and an ionic conductivity of 9.10 mS/cm at a temperature of 25 °C. Additionally, the use of cellulose in GPEs does not affect the electrochemical window. When the pure PAM-based GPE was compared to the CSC/PAM-based GPE, the biocomposites demonstrated electrochemical stability for a cycle life of over 200 cycles in the ZIB application. [ABSTRACT FROM AUTHOR]

Due to some specific properties of adiponitrile (ADN) including high oxidative stability and high flash point, it is proposed as co‐solvent with an ionic liquid (IL) as a promising electrolyte solvent for application in magnesium batteries. Herein, we report a flexible film of gel polymer electrolyte (GPE) comprising a polymer poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVdF‐HFP) in which a liquid electrolyte of Mg‐trifluoromethane sulfonate (Mg‐triflate) in the mixture of ADN:IL (1‐ethyl‐3‐methylimidazolium triflate, EMITf) is immobilized for use in Mg‐batteries. The structural/morphological properties of the GPE film have been characterized via different physical techniques. The high ionic conductivity (σRT = 5.9 mS cm−1), wide potential range of oxidative stability (~4.18 V vs. Mg/Mg2+), high Mg‐ion transport number (tMg2+ = 0.67) and thermal stability up to ~160°C ascertain the compatibility of electrolyte film in magnesium batteries with high voltage cathode materials. The comparative studies of the interfacial‐stability and Mg‐stripping/plating tests on the two symmetrical cells with Mg and Mg/MWCNTs nanocomposite electrodes show the improved reversibility of the electrolyte film with Mg‐MWCNTs powder as anode material, compared with pure Mg‐powder. The overall results indicate that the GPE based on binary solvent mixture ADN:IL is high performance flexible electrolyte for Mg‐batteries with Mg‐MWCNTs powder as anode material. [ABSTRACT FROM AUTHOR]

Membrane separation technology is one of the most widely studied methods for wastewater treatment. This paper is based on the non-solvent-induced phase separation (NIPS) method, which is combined with phase-field simulation to develop a fluid model for the volume fraction of tetrameric polyvinylidene fluoride (PVDF).In this paper, DMSO, DMAc and DMF are used as solvents, and pure water is used as a gel bath to simulate the relevant parameters of PVDF membrane; and PVP and LiCl are used as additives, and DMF and DMAc are used as solvents for the two-by-two combinations, and by calculating the relevant parameters of the PVDF quaternary membrane system, comparing and verifying the simulation results through experiments. results show that: the different solvents on the PVDF membrane in the order of DMSO > DMAc > DMF; additive LiCl system, the polymer diffusion rate in the polymer solution layer are faster than the PVP system. However, the top layer of the polymer solution layer in the PVP system is relatively flat, while the top layer of the polymer solution layer in the additive LiCl system is more undulating or even broken, indicating that LiCl has a greater influence on the membrane than PVP. [ABSTRACT FROM AUTHOR]

Since the last decade, the need for deformable electronics exponentially increased, requiring adaptive energy storage systems, especially batteries and supercapacitors. Thus, the conception and elaboration of new deformable electrolytes becomes more crucial than ever. Among diverse materials, gel polymer electrolytes (hydrogels, organogels, and ionogels) remain the most studied thanks to the ability to tune the physicochemical and mechanical properties by changing the nature of the precursors, the type of interactions, and the formulation. Nevertheless, the exploitation of this category of electrolyte as a possible commercial product is still restrained, due to different issues related to the nature of the gels (ionic conductivity, evaporation of filling solvent, toxicity, etc.). Therefore, this review aims to resume different strategies to tailor the properties of the gel polymer electrolytes as well as to provide recent advancements in the field toward the elaboration of deformable batteries and supercapacitors. [ABSTRACT FROM AUTHOR]

The progress in polymer science and nanotechnology yields new colloidal and macromolecular objects and their combinations, which can be defined as complex polymer materials. The complexity may include a complicated composition and architecture of macromolecular chains, specific intermolecular interactions, an unusual phase behavior, and a structure of a multi-component polymer-containing material. Determination of a relation between the structure of a complex material, the structure and properties of its constituent elements, and the rheological properties of the material as a whole is the subject of structural rheology—a valuable tool for the development and study of novel materials. This work summarizes the author's structural–rheological studies of complex polymer materials for determining the conditions and rheo-manifestations of their micro- and nanostructuring. The complicated chemical composition of macromolecular chains and its role in polymer structuring via block segregation and cooperative hydrogen bonds in melt and solutions is considered using tri- and multiblock styrene/isoprene and vinyl acetate/vinyl alcohol copolymers. Specific molecular interactions are analyzed in solutions of cellulose; its acetate butyrate; a gelatin/carrageenan combination; and different acrylonitrile, oxadiazole, and benzimidazole copolymers. A homogeneous structuring may result from a conformational transition, a mesophase formation, or a macromolecular association caused by a complex chain composition or specific inter- and supramolecular interactions, which, however, may be masked by macromolecular entanglements when determining a rheological behavior. A heterogeneous structure formation implies a microscopic phase separation upon non-solvent addition, temperature change, or intense shear up to a macroscopic decomposition. Specific polymer/particle interactions have been examined using polyethylene oxide solutions, polyisobutylene melts, and cellulose gels containing solid particles of different nature, demonstrating the competition of macromolecular entanglements, interparticle interactions, and adsorption polymer/particle bonds in governing the rheological properties. Complex chain architecture has been considered using long-chain branched polybutylene-adipate-terephthalate and polyethylene melts, cross-linked sodium hyaluronate hydrogels, asphaltene solutions, and linear/highly-branched polydimethylsiloxane blends, showing that branching raises the viscosity and elasticity and can result in limited miscibility with linear isomonomer chains. Finally, some examples of composite adhesives, membranes, and greases as structured polymeric functional materials have been presented with the demonstration of the relation between their rheological and performance properties. [ABSTRACT FROM AUTHOR]

Cover Photograph: Shown on the cover are 3D printed lithium‐containing ceramic electrodes used in the study on 3D printed gel polymer electrolyte containing highly ordered, mesoporous silica‐based sieve as filler. The fired electrodes retain the hexagonal printed structure. The surfaces are very smooth, and each filament shows a very dense structure, ensuring a high material loading density. Seehttps://ceramics.onlinelibrary.wiley.com/doi/10.1111/jace.19863for more information.. [Extracted from the article]

The current work reports on tailoring of 3D printed gel polymer electrolyte (GPE) employing poly(vinylidene fluoride‐co‐hexafluoropropylene) P(VdF‐HFP) as the host matrix and mesoporous Santa Barbara Amorphous‐15 (SBA‐15) mesoporous sieve as ceramic filler. Further, this work envisages an investigation on its physicochemical properties, thermal shrinkage behavior, and electrochemical performance. An effort has been undertaken to formulate 3D printable P(VdF‐HFP)/SBA‐15 composite‐based GPE ink with suitable rheological properties. The breath figure method is followed to investigate the influence of 1‐methyl‐2‐pyrrolidinone (NMP)/tetrahydrofuran (THF) mixture as a solvent on the porosity of 3D printed GPE, through which enhanced porosity is evident from scanning electron microscopy (SEM) analysis. The morphological analysis further confirms the hybrid porous structure facilitated by the addition of SBA‐15 into the P(VdF‐HFP) matrix. The 3D printed P(VdF‐HFP)/SBA‐15 (10%) composite‐based GPE shows promising ionic conductivity in the order of 0.2 × 10−4 S/cm at room temperature and demonstrates excellent dimensional thermal stability up to 175°C. The electrochemical measurement of 3D printed GPE is tested separately using 3D printed cathode half‐cell (3D printed LFP vs. Li+) and 3D printed anode half cell (3D printed LTO vs. Li+) with GPE as separator. Further, also tested with conventionally prepared electrode and the coin cell studies show discharge capacity of 3D printed P(VdF‐HFP)/SBA‐15 (10%) composite‐based GPE is comparable to commercial celgard separator. All these features speculate that the 3D printed fabricated in the current work may find potential application in lithium‐ion battery. [ABSTRACT FROM AUTHOR]

[Display omitted] Solid polymer electrolytes (SPEs) are effective solutions for the development of high-performance and flexible lithium metal batteries (LMBs). However, the key problems of SPEs including low ionic conductivity and inability to repair damage have hindered their industrialization process. In this work, a three-dimensional (3D) cross-linked network gel polymer electrolyte (CNGPE) is designed. The addition of deep eutectic solvent (DES) improves the ionic conductivity of CNGPE. The hydrogen bonds and dynamic disulfide bonds in the 3D cross-linked network endow CNGPE rapid self-healing ability at ambient temperature. In addition, the addition of lithium difluoro(oxalato)borate (LiDFOB) and lithium nitrate (LiNO 3) helps to form a stable solid electrolyte interface (SEI). Due to the ingenious design, the Li/CNGPE/Li symmetrical cell exhibits excellent interface stability and no short circuit occurs for more than 800 h. The assembled LiFePO 4 /CNGPE/Li cell exhibits a discharge specific capacity of 126 mAh g−1 after 960 cycles at 0.5C. This work has shown that the self-healing gel polymer electrolyte containing DES provides an effective and feasible method for the development of high-performance LMBs. [ABSTRACT FROM AUTHOR]

Background: Coincidence of the treatment and imaging isocenter coordinates is required to safely perform small‐margin treatments, such as stereotactic radiosurgery of multiple brain metastases. A comprehensive and direct methodology for verifying concordance of kilovoltage cone‐beam computed tomography (kV‐CBCT) and treatment coordinates using an x‐ray CT‐based polymer gel dosimeter (dGEL) and onboard kV‐CBCT was previously reported. Using this methodology, we tested the ability of a new commercially available x‐ray CT‐based polymer dGEL with a rapid response to provide efficient quality assurance (QA). Purpose: The aim of this study was to evaluate the robustness of the three‐dimensional geometric QA methodology using dGEL. Methods: The dGEL were commercially manufactured. The prescribed dose for each field was determined by visually identifying the 5, 10, and 20 Gy isodose lines. A linear accelerator was used to irradiate the gels with seven non‐coplanar beams. An in‐house analysis program was used to identify the beam axes and treatment isocenter in kV‐CBCT coordinates by processing the pre‐ and post‐irradiation CBCT images. The impact of the radiation dose on the test reproducibility was examined, and the detectability of an intentional geometric error was assessed. Results: The treatment isocenter was within 0.4 mm of the imaging isocenter for all radiation doses. The residual error of the test with the intentional error was within 0.2 mm. The analysis and image quality variations for a single dGEL introduced displacement errors less than 0.3 mm. Conclusions: The test assessed the coincidence of treatment and kV‐CBCT isocenter coordinates and detected errors with high robustness. Even for a 10 Gy dose, the test yielded results comparable with those obtained using higher radiation doses owing to the rapid response of the dGEL dosimeter. [ABSTRACT FROM AUTHOR]

A theoretical framework is established for the gel diffusiophoresis of a spherical colloidal particle moving through an uncharged dilute porous polymer gel medium when an electrolyte concentration gradient field is applied. The network of cross-linked polymer segments is treated as a porous skeleton containing an electrolyte solution using the Brinkman–Debye–Bueche model. We derive a general expression for the gel-diffusiophoretic mobility of a charged spherical colloidal particle. Based on this general mobility expression, we farther derive a closed-form approximate expression for the gel-diffusiophoretic mobility of a weakly charged spherical particle correct to the second order of the particle's zeta potential. The obtained mobility expression depends on the Debye–Hückel parameter and the Brinkmann parameter. [ABSTRACT FROM AUTHOR]

Polymer gel was widely used as water shutoff agent in mature oil fields. And the results of single-phase plugging experiments show that the plugging rate of the polymer gel to the oil phase is lower than that of the water phase. However, the disproportionate permeability reduction (DPR) mechanism of polymer gels still remains controversial. In this paper, we used four gel formulations including polyethyleneimine (PEI) and phenol-formaldehyde crosslinked gel with and without adding laponite to investigate the effect of gel elastic property on the water shutoff mechanism. The result of sand pack flooding experiments shown that the gel with higher elastic modulus has better effects on decreasing water cut and increasing oil recovery. After adding laponite, the elastic modulus of phenol-formaldehyde crosslinked gel increased from 64.2 Pa to 192 Pa, and the elastic modulus of PEI crosslinked gel increased from 27.4 Pa to 36.5 Pa. Compared to the phenol-formaldehyde-HAPM gel, the oil recovery of laponite-phenol-formaldehydeHPAM gel increased by 5.2% and the maximum water cut decreased by 8.3%. Besides, comparing with PEI-HPAM gel, the oil recovery of laponite-PEI-HPAM gel increased by 2.7% and the water cut dropped by 27.8%. In the meanwhile, the laponite-phenol-formaldehyde-HPAM gel with higher elastic modulus obviously swells in the formation water but almost remains constant in oil at 105(C. The mass of gel soaked in the formation water increased from 42 g to 96 g and the gel volume increased by 300% within 48 hours. This study improves the understanding of the DPR mechanism of polymer gel for water shutoff. [ABSTRACT FROM AUTHOR]

This study addresses the critical challenge of excessive water production in mature oil and gas reservoirs. It focuses on the effectiveness of polymer gel injection into porous media as a solution, with an emphasis on understanding its impact at the pore scale. A step-wise Lattice Boltzmann Method (LBM) is employed to simulate polymer gel injection into a 2D Berea sample, representing a realistic porous media. The non-Newtonian, time-dependent characteristics of polymer gel fluid necessitate this detailed pore-scale analysis. Validation of the simulation results is conducted at each procedural step. The study reveals that the methodology is successful in predicting the effect of polymer gel on reducing permeability as the gel was mainly formed in relatively larger pores, as it is desirable for controlling water cut. Mathematical model presented in this study accurately predicts permeability reductions up to 100% (complete blockage). In addition, simulations conducted over a wide range of gelation parameters, TD_factor from 1 to 1.14 and Threshold between 0.55 and 0.95, revealed a quadratic relationship between permeability reduction and these parameters. The result of this research indicates LBM can be considered as promising tool for investigating time-dependant fluids on porous media. [ABSTRACT FROM AUTHOR]

Zn–air batteries (ZABs) are a promising technology; however, their commercialization is limited by challenges, including those occurring in the electrolyte, and thus, gel polymer electrolytes (GPEs) and hydrogels have emerged as substitutes for traditional aqueous electrolytes. In this work, PVA/PAA membranes were synthesized by the solvent casting method and soaked in 6 M KOH to act as GPEs. The thickness of the membrane was modified (50, 100, and 150 μm), and after determining the best thickness, the membrane was modified with synthesized SiO2 nanospheres and multi-walled carbon nanotubes (CNTs). SEM micrographs revealed that the CNTs displayed lengths of tens of micrometers, having a narrow diameter (95 ± 7 nm). In addition, SEM revealed that the SiO2 nanospheres had homogeneous shapes with sizes of 110 ± 10 nm. Physicochemical experiments revealed that SiO2 incorporation at 5 wt.% increased the water uptake of the PVA/PAA membrane from 465% to 525% and the ionic conductivity to 170 mS cm−1. The further addition of 0.5 wt.% CNTs did not impact the water uptake but it promoted a porous structure, increasing the power density and the stability, showing three-times-higher rechargeability than the ZAB operated with the PVA/PAA GPE. [ABSTRACT FROM AUTHOR]

An alternative synthetic pathway was proposed for the optimization of synthesis to find a better correlation between the swelling and elasticity of hyaluronic acid-interpenetrated gels via temperature regulation. An experimental design methodology was presented for the synthesis of polyacrylamide/poly(acrylic acid sodium salt)/hyaluronic acid, PAAm/PSA/HyA, gels by modifying the one-pot procedure using free radical crosslinking copolymerization of AAm with the addition of anionic linear PSA chains in the presence of various amount of HyA, ranging between 0.05% and 0.20% (w/v). Semi-interpenetrated polymer network (IPN)-structured gels were designed with tunable elasticity, in which the extent of covalent crosslinking interactions is controlled by polymerization temperature ranging between −18 and 45 °C. Depending on the HyA content added in the synthesis and the polymerization temperature, the swelling ratio could be controlled. The addition of 0.05% (w/v) HyA increased the swelling of semi-IPNs, while the elastic modulus increased with increasing HyA content and decreased with the polymerization temperature. PAAm/PSA/HyA semi-IPNs showed the typical pH-sensitive swelling of anionic gels, and the swelling reached a maximum at a pH of 11.2. PAAm/PSA/HyA gels were tested for the removal of methyl violet from wastewater. Adsorption kinetics were shown to be well-fitted with the pseudo-second-order model using linear and nonlinear regression analysis. With the clear relationship between increased modulus and composition, this study enabled the fine-tuning of semi-IPN interactions by varying the polymerization temperature. [ABSTRACT FROM AUTHOR]

The rapid expansion of flexible and wearable electronics has necessitated a focus on ensuring their safety and operational reliability. Gel polymer electrolytes (GPEs) have become preferred alternatives to traditional liquid electrolytes, offering enhanced safety features and adaptability to the design requirements of flexible lithium-ion batteries. This review provides a comprehensive and critical overview of recent advancements in GPE technology, highlighting significant improvements in its physicochemical properties, which contribute to superior long-term cycling stability and high-rate capacity compared with traditional organic liquid electrolytes. Special attention is given to the development of smart GPEs endowed with advanced functionalities such as self-protection, thermotolerance, and self-healing properties, which further enhance battery safety and reliability. This review also critically examines the application of GPEs in high-energy cathode materials, including lithium nickel cobalt manganese (NCM), lithium nickel cobalt aluminum (NCA), and thermally stable lithium iron phosphate (LiFePO4). Despite the advancements, several challenges in GPE development remain unresolved, such as improving ionic conductivity at low temperatures and ensuring mechanical integrity and interfacial compatibility. This review concludes by outlining future research directions and the remaining technical hurdles, providing valuable insights to guide ongoing and future efforts in the field of GPEs for lithium-ion batteries, with a particular emphasis on applications in high-energy and thermally stable cathodes. [ABSTRACT FROM AUTHOR]

Despite the numerous ongoing research studies in the area of conducting polymer-based electrode materials for supercapacitors, the implementation has been inadequate for commercialization. Further understanding is required for the design and synthesis of suitable materials like conducting polymer-based gels as electrode materials for supercapacitor applications. Among the polymers, conductive polymer gels (CPGs) have generated great curiosity for their use as supercapacitors, owing to their attractive qualities like integrated 3D porous nanostructures, softness features, very good conductivity, greater pseudo capacitance, and environmental friendliness. In this review, we describe the current progress on the synthesis of CPGs for supercapacitor applications along with their morphological behaviors and thermal properties. We clearly explain the synthesis approaches and related phenomena, including electrochemical approaches for supercapacitors, especially their potential applications as supercapacitors based on these materials. Focus is also given to the recent advances of CPG-based electrodes for supercapacitors, and the electrochemical performances of CP-based promising composites with CNT, graphene oxides, and metal oxides is discussed. This review may provide an extensive reference for forthcoming insights into CPG-based supercapacitors for large-scale applications. [ABSTRACT FROM AUTHOR]

We report the synthesis of novel cobalt complexes-based catalysts designed for the oscillatory Belousov–Zhabotinsky (BZ) reaction. For the first time, we introduce cobalt complex-based self-oscillating gels that demonstrate autonomous color oscillations within a BZ reagent solution, functioning without the need for any external stimuli. We created acrylamide-based self-oscillating gels containing immobilized tris(2,2′-bipyridine)cobalt(II) or tris(1,10-phenanthroline)cobalt(II) complexes and gels containing covalently bound (5-acrylamido-1,10-phenanthroline)bis(2,2′-bipyridine)cobalt(II), (5-acrylamido-1,10-phenanthroline)bis(1,10-phenanthroline) cobalt(II), or tris(5-acrylamido-1,10-phenanthroline)cobalt(II) complexes. When the BZ reaction takes place within the gels, it results in the observation of moving chemical waves and reversible color changes. We believe that Co-complexes-based self-oscillating gels have potential applications in the design of soft actuators and chemical devices for signal processing. [ABSTRACT FROM AUTHOR]