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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]

[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]

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]

Polymer electrolytes play a crucial role in advancing rechargeable magnesium batteries (RMBs) owing to their exceptional characteristics, including high flexibility, superior interface compatibility, broad electrochemical stability window, and enhanced safety features. Despite these advantages, research in this domain remains nascent, plagued by single preparation approaches and challenges associated with the compatibility between polymer electrolytes and Mg metal anode. In this study, we present a novel synthesis strategy to fabricate a glycerol α,α′‐diallyl ether‐3,6‐dioxa‐1,8‐octanedithiol‐based composite gel polymer electrolyte supported by glass fiber substrate (GDT@GF CGPE) through anion modification and thiol‐ene click chemistry polymerization. The developed route exhibits novelty and high efficiency, leading to the production of GDT@GF CGPEs featuring exceptional mechanical properties, heightened ionic conductivity, elevated Mg2+ transference number, and commendable compatibility with Mg anode. The assembled modified Mo6S8||GDT@GF||Mg cells exhibit outstanding performance across a wide temperature range and address critical safety concerns, showcasing the potential for applications under extreme conditions. Our innovative preparation strategy offers a promising avenue for the advancement of polymer electrolytes in high‐performance rechargeable magnesium batteries, while also opens up possibilities for future large‐scale applications and the development of flexible electronic devices. [ABSTRACT FROM AUTHOR]

This research presents the development of niobium (Nb)‐doped titania (TiO2)/reduced graphene oxide (rGO) nanocomposites (NTR NCs) for dye‐sensitized solar cells (DSSCs). The novelty lies in two aspects: introducing Nb (V) ions into TiO2/rGO nanocomposites via an in‐situ sol‐gel method with doping concentrations from 1.0 to 3.0 mol %, and fabricating photoanodes using the doctor blade technique, sensitized with a Co2+/Co3+‐based PEO‐PEG polymer gel electrolyte‐assisted D‐π‐A carbazole metal‐free (SK3) dye. Detailed investigations into the optoelectrical, structural, and morphological properties were conducted using various spectral and analytical tools. Notably, DSSCs based on Nb‐doped TiO2/rGO nanocomposites with 2.0 mol % Nb (NTR‐2) achieved a remarkable solar efficiency (η) of 5.48 % under AM 1.5 solar simulation, significantly outperforming devices based on bare TiO2 nanoparticles and undoped TiO2/rGO NCs by factors of 4.15 and 2.97, respectively. The substantial enhancement in photovoltaic performance is attributed to superior charge transfer properties and higher carrier density, as revealed by electrochemical impedance spectroscopy (EIS) and Mott‐Schottky (M–S) analysis. Nb‐doping results in an energetic surface nature, improved optical absorption, and reduced charge transfer resistance, collectively boosting the overall efficiency of DSSCs. This work underscores the potential of Nb‐doped TiO2/rGO NCs as effective photoanode materials in enhancing DSSC performance. [ABSTRACT FROM AUTHOR]

It remains a great challenge to achieve strong and reversible hydrogel adhesion. Hydrogel adhesives also suffer from poor environmental stability due to dehydration. To overcome these problems, here reversible adhesive gels are designed using a new switching mechanism and new solvent. For the first time, the study observes UCST (upper critical solution temperature)‐type thermosensitive behaviors of poly(benzyl acrylate) (PBnA) polymer and gel in menthol:thymol deep eutectic solvents (DESs). The temperature‐induced phase transition allows adjusting cohesive force, and hence adhesion strength of PBnA gels by temperature. To further improve the mechanical and adhesion properties, a peptide crosslinker is used to allow energy dissipation when deforming. The resulting eutectogel exhibits thermal reversible adhesion with a high switching ratio of 14.0. The adhesion strength at attachment state reaches 0.627 MPa, which is much higher than most reversible adhesive hydrogels reported before. The low vapor pressure of DES endows the gel excellent environmental stability. More importantly, the gel can be repeatedly switched between attachment and detachment states. The strong and reversible gel adhesive is successfully used to design soft gripper for the transport of heavy cargos and climbing robot capable of moving on vertical and inverted surface in a manner similar to gecko. [ABSTRACT FROM AUTHOR]

Gel polymer electrolytes (GPEs) hold great promise for lithium (Li) metal batteries (LMBs). Nevertheless, a critical challenge lies in reducing the thickness of GPEs while maintaining their mechanical integrity to achieve high‐energy‐density LMBs. Additionally, protecting the Li metal anode via electrolyte engineering in GPEs remains demanding. Herein, an innovative ultrathin (1 µm‐thick) yet robust GPE developed using an in situ curing technique, featuring a nanofibrous, exceptionally strong polyethylene separator is presented. The unique microstructure, interfacial conformability, and ultrahigh mechanical robustness of the ultrathin polyethylene separator are thoroughly verified. Enhanced ionic association within the GPE is achieved due to the strong affinity of electrolyte solvent with the fluorinated polymer network, as confirmed by large‐scale molecular dynamics simulations. The optimized solvation structure with high contact ion pairs and aggregate fractions contributes to forming an anion‐derived inorganic‐rich solid electrolyte interphase (SEI), thereby protecting the lithium anode. Benefiting from the ultrahigh robustness of GPE and the excellent interfacial stability, the Li metal full cell with a high mass loading LiNi0.8Co0.1Mn0.1O2 cathode (≈17.3 mg cm−2) and thin Li foil anode (50 µm) demonstrates 91% capacity retention after 200 cycles. This design demonstrates a feasible approach toward the practical quasi‐solid‐state LMBs. [ABSTRACT FROM AUTHOR]

Visualizing the network of a solvent‐swollen polymer gel remains problematic. To address this challenge, open transmission electron microscopy (TEM) was applied to thin gel films permeated by a nonvolatile ionic liquid. The targeted physical gels were prepared by cooling concentrated solutions of poly(ethylene glycol) in 1‐ethyl‐3‐methyl imidazolium ethyl sulfate [EMIM][EtSO4]. During the cooling, gelation occurred by a frustrated crystallization of the dissolved polymer, leading to a percolated, solvent‐permeated semicrystalline network in which nanoscale polymer crystals acted as crosslinks. Crystalline features ranging from ~5 to ~200 nm were observed, with the visible network strands dominantly consisting of long curvilinear crystallites of ~15–20 nm diameter. Nascent spherulites irregularly decorated the network, creating a complex structural hierarchy that complicated analyses. Lacking diffraction contrast, TEM did not visualize the many disordered, fully solvated PEG chains present in the voids between crystals. Recognizing that a network's three dimensionality is ambiguous when assessed through two‐dimensional microscopy projections, a small gel region was studied by TEM tomography, revealing a nearly isotropic three‐dimensional arrangement of the curvilinear crystallites, which displayed remarkably uniform cylindrical cross sections. [ABSTRACT FROM AUTHOR]

In situ polymerization of 1,3-dioxolane (DOL) based liquid precursor as gel polymer electrolyte (GPE) is a promising strategy to prepare solid-state lithium metal batteries. However, the poor structural stability and low lithium ion transference number (tLi+) of the linear poly(1,3-dioxolane) (PDOL) GPE limit its commercial application. Herein, a cross-linked GPE is prepared by lithium salt initiated in situ thermal polymerization of DOL and glycerol triglycidyl ether (GTE) monomers. A fluoroethylene carbonate (FEC) liquid plasticizer is further introduced to promote the dissociation of lithium salts, and the obtained PDOL–FEC–GTE composite electrolyte exhibits ionic conductivity of 2.1 × 10−4 S cm−1, tLi+ of 0.58 and wide electrochemical stability window of 5.1 V. Li‖Li symmetric cell is stably operated for 790 h at 1.0 mA cm−2 and 1.0 mA h cm−2. LiFePO4‖PDOL–FEC–GTE‖Li full cell delivers a discharge specific capacity of 120.8 mA h g−1 after 200 cycles at a current rate of 1C with a capacity retention of 84.1%. This work provides new ideas for accelerating the practical application of solid-state lithium metal batteries. [ABSTRACT FROM AUTHOR]

In 1952, Alan Turing accomplished a pioneering theoretical study to show that the coupling of nonlinear chemical reactions and diffusion leads to the instability of spatially homogeneous states. The activator and inhibitor are synthesized as intermediates of the reaction system in the Turing model. Turing found that spatially periodic stationary concentration patterns are spontaneously generated when the diffusion coefficient of the activator is lower than that of the inhibitor. The first experimental realization of the Turing pattern was achieved in 1990 in a chlorite-iodide-malonic acid (CIMA) reaction system. Iodide and chlorite anions act as the activator and inhibitor of this reaction system, respectively. Although there is no significant difference in the diffusion coefficient of iodide and chlorite anions, the Turing pattern was generated because starch was added to the gel reactor to enhance the color tone. This formed a complex with iodide to inhibit its diffusion to satisfy the condition for the Turing instability. Several examples were found after this finding. We focused on the high affinity of quaternary alkyl ammonium cations to iodide. The CIMA reaction was performed in an open gel reactor by adding a quaternary alkyl ammonium cationic surfactant. In addition, the polymer gel consists of the quaternary alkyl ammonium group as the side chain was utilized for the open gel reactor. The micelles of the surfactants and the polymer gels trapped iodide in their vicinity as a counter anion to lower the effective diffusivity to satisfy the condition for the Turing instability. [ABSTRACT FROM AUTHOR]

Flexible wearable supercapacitors based on hydrogel electrolyte are considered as flexible energy storage device with great potential. However, polymer gel electrolytes contain a large number of water molecules, which can easily freeze at sub‐zero temperatures, thus severely inhibiting ion transport. The ionic conductivity, cyclic stability and mechanical properties of gel electrolytes decrease at low temperatures (below −25°C), which seriously hinders the application of flexible wearable supercapacitors. In order to improve the mechanical properties and ensure the excellent ionic conductivity of the electrolyte, a freezing‐resistant gel electrolyte constructed by supramolecular self‐assembly, which has a wide temperature range from 25 to −80°C, stable ionic conductivity and ultra‐high mechanical strength. Low‐temperature‐resistant gel electrolytes, called flexible supercapacitor‐SBMA‐co‐PVA‐AA/CaCl2 (FSAPC), have been designed and prepared by molecular‐scale supramolecular self‐assembly of rigid [2‐(methacryloyloxy)ethyl]dimethyl(3‐sulfopropyl) polymer chains and flexible poly(vinyl alcohol) polymer chains, and the test results showed that the gel electrolyte ‐SBMA‐co‐PVA‐AA/CaCl2 (PSAPC) has excellent conductivity of 34.07 mS cm−1 at 25°C, the flexible supercapacitor has a specific capacity of 8.57 Wh kg−1, and the capacity retention rate is 91.2% even after 5000 cycles at −25°C, excellent conductivity at −25°C for 31.88 mS cm−1 and at −80°C for 35.34 mS cm−1. The potential applications of the amphiphilic ionic gel electrolyte in the industrial development of low‐temperature resistant supercapacitors are noteworthy. [ABSTRACT FROM AUTHOR]

Objective. To develop and benchmark a novel 3D dose verification technique consisting of polymer gel dosimetry (PGD) with cone-beam-CT (CBCT) readout through a two-institution study. The technique has potential for wide and robust applicability through reliance on CBCT readout. Approach. Three treatment plans (3-field, TG119-C-shape spine, 4-target SRS) were created by two independent institutions (Institutions A and B). A Varian Truebeam linear accelerator was used to deliver the plans to NIPAM polymer gel dosimeters produced at both institutions using an identical approach. For readout, a slow CBCT scan mode was used to acquire pre- and post-irradiation images of the gel (1 mm slice thickness). Independent gel analysis tools were used to process the PGD images (A: VistaAce software, B: in-house MATLAB code). Comparing planned and measured doses, the analysis involved a combination of 1D line profiles, 2D contour plots, and 3D global gamma maps (criteria ranging between 2%1 mm and 5%2 mm, with a 10% dose threshold). Main results. For all gamma criteria tested, the 3D gamma pass rates were all above 90% for 3-field and 88% for the SRS plan. For the C-shape spine plan, we benchmarked our 2% 2 mm result against previously published work using film analysis (93.4%). For 2%2 mm, 99.4% (Institution A data), and 89.7% (Institution B data) were obtained based on VistaAce software analysis, 83.7% (Institution A data), and 82.9% (Institution B data) based on MATLAB. Significance. The benchmark data demonstrate that when two institutions follow the same rigorous procedures gamma passing rates up to 99%, for 2%2 mm criteria can be achieved for substantively different treatment plans. The use of different software and calibration techniques may have contributed to the variation in the 3D gamma results. By sharing the data across institutions, we observe the gamma passing rate is more consistent within each pipeline, indicating the need for standardized analysis methods. [ABSTRACT FROM AUTHOR]

The advancement of implantable biomedical devices (IMDs) hinges on the development of biocompatible solid-state electrolytes with outstanding electrochemical performance, safety, and reliability for flexible solid-state supercapacitors. This study focuses on the development of gel polymer electrolytes (GPEs) using polyvinyl alcohol (PVA) and potassium chloride (KCl). The GPEs obtained were subjected to comprehensive characterization using a diverse range of techniques to evaluate their spectral features, morphological properties, thermal and mechanical performance, biocompatibility, ionic conductivity, and cyclic stability. What distinguishes our research is its comprehensive exploration of the profound impact of varying PVA molecular weights and PVA/KCl weight ratios on the ionic conductivity and thermal characteristics of these gels. Notably, we observed a decrease in ionic conductivity with increasing PVA molecular weight, whereas an increase in salt concentration under the same molecular weight led to higher ionic conductivity. In particular, the optimal gel electrolyte with a molecular weight (Mw) of 195,000 g/mol and a PVA/KCl weight ratio of 1/2 demonstrated a promising ionic conductivity of 3.48 ± 0.25 mS/cm. Even after 5000 cycles, it retained 88% of its initial specific capacitance. Our findings reveal that the GPEs exhibit remarkable mechanical robustness alongside unparalleled ionic conductivity, characterized by minimal interfacial resistance. Moreover, these gel electrolytes exhibit remarkable biocompatibility, evident in a cell viability test where 72.3% of cells remained unaffected after a 72-h exposure to PVA/KCl. These findings present a promising avenue towards the fabrication of stable and high-performance biocompatible gel polymer electrolytes which can be used in solid-state supercapacitors, thereby laying the foundation for their integration into flexible, safer, and wearable bio-electronics. [ABSTRACT FROM AUTHOR]

Dye-sensitized solar cells were fabricated with a polyethylene oxide (PEO)-based quasi-solid (gel) electrolyte consisting of the ionic liquid 1-hexil-3-methylimidazoliym iodide (HMII), and tetrapropyl ammonium iodide (Pr4N+I−) as the two iodide salts with two dissimilar cations. Titanium dioxide powder (TiO2) (P-25) was added to the polymer electrolyte to enhance the iodide ion conductivity further by the nanofiller effect. The electrolyte and the solar cells were characterized by ionic conductivity and impedance measurements, DC polarization test, and current-voltage measurements. The maximum ionic conductivity of 6.95 × 10−3 S cm−1 at 30 °C was exhibited by the electrolyte composition with a 5 wt% TiO2 nanofiller concentration, and the activation energy of this electrolyte was 0.181 eV. The solar cell with this conductivity-optimized gel electrolyte had the highest short-circuit photocurrent of 8.72 mA cm−2 and the highest efficiency of 4.04% with an open-circuit voltage of 685.4 V and a fill factor of 67.6%. The addition of TiO2 nanofiller to the PEO-based gel polymer electrolyte has increased the electron recombination lifetime in the TiO2 photoanode from 2.23 ms for the TiO2 nanofiller-free electrolyte to 33.84 ms for the filler-added electrolyte. The enhancement of the solar cell efficiency is attributed to the mixed cation effect and the diffusion-mediated ionic conductivity increase due to the presence of the TiO2 nanofiller. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries (LIBs) benefit from an effective electrolyte system design in both terms of their safety and energy storage capability. Herein, a series of precursor membranes with high porosity were produced using electrospinning technology by mixing PVDF and triblock copolymer (PS-PEO-PS), resulting in a porous structure with good interconnections, which facilitates the absorbency of a large amount of electrolyte and further increases the ionic conductivity of gel polymer electrolytes (GPEs). It has been demonstrated that post-cross-linking of the precursor membranes increases the rigidity of the nanofibers, which allows the polymer film to be dimensionally stable up to 260 °C while maintaining superior electrochemical properties. The obtained cross-linked GPEs (CGPEs) showed high ionic conductivity up to 4.53×10−3 S·cm−1. With the CGPE-25, the assembled Li/LiFePO4 half cells exhibited good rate capability and maintained a capacity of 99.4% and a coulombic efficiency of 99.3% at 0.1 C. These results suggest that the combination of electrospinning technique and post-cross-linking is an effective method to construct polymer electrolytes with high thermal stability and steadily decent electrochemical performance, particularly useful for Lithium-ion battery applications that require high-temperature usage. [ABSTRACT FROM AUTHOR]

Recent advancements in medical dosimetry have significantly improved the precision and effectiveness of radiation therapy by accurately quantifying absorbed doses from ionizing radiation. In the past, conventional one-dimensional and two-dimensional dosimeters were commonly used, but recent years have seen a surge in interest in 3D dosimeters for complex radiation therapies. This review aims to elucidate the applications of 3D polymer gel dosimeters in radiation therapies, covering diverse radiation and energy fields. Utilizing an extensive search strategy across various electronic databases, the review synthesizes insights from recent studies on polymer gel dosimeters, exploring their properties and applications in ultrasound, optical coherence tomography, magnetic resonance imaging, and computed tomography. Furthermore, the review investigates the consideration of Monte Carlo simulations in modeling dosimeter applications in radiation therapy, examining specific parameters affecting dosimeter performance. It provides a comprehensive synthesis of available data over the past decade, shedding light on the medical applications of 3D polymer gel dosimeters and their potential limitations. Finally, the review discusses challenges in widespread implementation and future directions, emphasizing the need for further research on novel gel dosimeters and the incorporation of nanoparticles to enhance sensitivity and functionality in medical dosimetry. [ABSTRACT FROM AUTHOR]

The current work presents a new structure based on Au/PVA/SiO2/p-Si/Al that has not been studied before. An aqueous solution of polyvinyl alcohol (PVA) polymer gel was deposited on the surface of SiO2/Si using the spin-coating technique. The silicon wafer was left to be oxidized in a furnace at 1170 k for thirty minutes, creating an interdiffusion layer of SiO2. The variations in the dielectric constant (Є′), dielectric loss (Є″), and dielectric tangent (tanδ) with the change in the frequency, voltage, and temperature were analyzed. The results showed an increase in the dielectric constant (Є′) and a decrease in the dielectric loss (Є″) and tangent (tanδ); thus, the Au/PVA/SiO2/p-Si/Al heterostructure has opened up new frontiers for the semiconductor industry, especially for capacitor manufacturing. The Cole–Cole diagrams of the Є″ and Є′ have been investigated at different temperatures and voltages. The ideality factor (n), barrier height (Φb), series resistance (Rs), shunt resistance (Rsh), and rectification ratio (RR) were also measured at different temperatures. [ABSTRACT FROM AUTHOR]

When encountering heavy oil reservoirs during drilling, due to the change in pressure difference inside the well, heavy oil will invade the drilling fluid, and drilling fluid will spill into the reservoir along the formation fractures, affecting the drilling process. A supramolecular polymer gel-based temporary plugging agent was prepared using acrylamide (AM), butyl acrylate (BA), and styrene (ST) as reacting monomers, N, N-methylenebisacrylamide (MBA) as a crosslinking agent, ammonium persulfate (APS) as an initiator, and poly(vinyl alcohol) (PVA) as a non-covalent component. A supermolecular polymer gel with a temperature tolerance of 120 °C and acid solubility of 90% was developed. The experimental results demonstrated that a mechanically robust, thermally stable supramolecular polymer gel was successfully synthesized through the copolymerization of AM, BA, and ST, as well as the in situ formation hydrogen bonding between poly (AM-co-BA-co-ST) and PVA, leading to a three-dimensional entangled structure. The gel-forming solution possessed excellent gelling performance even in the presence of a high content of salt and heavy oil, demonstrating superior resistance to salt and heavy oil under harsh reservoir conditions. High-temperature and high-pressure plugging displacement experiments proved that the supramolecular polymer gel exhibited high pressure-bearing capacity, and the blocking strength reached 5.96 MPa in a wedge-shaped fracture with a length of 30 cm. Furthermore, the dissolution rate of the supramolecular polymer gel was as high as 96.2% at 120 °C for 48 h under a 15% HCl solution condition. [ABSTRACT FROM AUTHOR]

Chemiluminescence in solution-based systems has been extensively studied for the chemical analysis of biomolecules. However, investigations into the control of chemiluminescence reactions in gel-based systems, which offer flexibility in reaction conditions (such as the softness of the reaction environment), have only recently begun in polymer materials, with limited exploration in low-molecular-weight gelator (LMWG) systems. In this study, we investigated the chemiluminescence behaviors in the gel states using LMWG systems and evaluated their applicability to fluorescent-dye-containing molecular organogel systems/oxidant-containing aqueous systems. Using diethyl succinate organogels composed of 12-hydroxystearic acid as a molecular organogelator, we examined the fluorescent properties of various fluorescent dyes mixed with oxidant aqueous solutions. As the reaction medium transitioned from the solution to the gel state, the emission color and chemiluminescence duration changed significantly, and distinct characteristics were observed, for each dye. This result indicates that the chemiluminescence behavior differs significantly between the solution and gel states. Additionally, visual inspection and dynamic viscoelastic measurements of the mixed fluorescent dye-containing molecular gels and oxidant-containing aqueous solutions confirmed that the chemiluminescence induced by the mixing occurred within the gel phase. Furthermore, the transition from the solution to the gel state may allow for the modulation of the mixing degree, thereby enabling control over the progression of the chemiluminescence reaction. [ABSTRACT FROM AUTHOR]

The Persistent development of quick and accessible readout tools promises to remove one of the barriers to the adoption of gel dosimetry as an applicable method in treatment clinics. Research and development in the imaging of polymer gel dosimeters continues with a focus on imaging in three dimensions. Each technique comes with its own set of advantages and challenges. In gel dosimeter research, efforts have been made to identify and develop alternative imaging methods for polymer gel dosimeters. Gel dosimeters can obtain reliable and accurate three-dimensional dose distributions from the correlation of different polymerization stages caused by radiation. The irradiated samples are examined using magnetic resonance imaging, optical computed tomography, and X-ray computed tomography. This research describes the basic features of imaging devices and the readout of irradiated dose data. Costs, availability, portability, contrast and resolution, high-resolution image reconstruction algorithm, and image reconstruction time of radiation absorption dosimeters for imaging devices are investigated in this research. This review has been done to present the mentioned imaging features and review the research done in this field for the optimal use of different imaging methods. [ABSTRACT FROM AUTHOR]

This paper reports hybrid gels combining a low‐molecular‐weight gelator (LMWG) and a photoinitiated crosslinked polymer gel (PG). The presence of the PG enhanced the stiffness and strength of the gel. The gels were loaded with heparin, and in the hybrid gel, the interpenetrated LMWG and PG networks somewhat restricted its release. In terms of stem cell growth, the hybrid gel significantly improved the performance of the PG because of the presence of the LMWG, which is an excellent substrate for stem cells in its own right. Furthermore, the presence of heparin in the hybrid gels also enhanced stem cell proliferation over longer timescales. Finally, these gels were photopatterned within the well‐plates used for tissue culture, with patterning helping control stem cell proliferation. In summary, these hybrid gels combine the advantageous features of both LMWG and PG: rheological performance is endowed by the PG with stem cell compatibility provided by the LMWG. The hybrid gels also control the release of the bioactive agent heparin and have capacity to be shaped and patterned. Patterned gels such as these, capable of directing stem cell growth, have potential in regenerative medicine. [ABSTRACT FROM AUTHOR]

Advancement of the voltage window with stringent safety concerns is an imperative strategy to enhance the energy densities and output power delivery of electrical double‐layer capacitors (EDLCs). Solid‐state, water‐in‐salt (WIS), and ionic liquid‐based electrolytes are attractive and ideal choices for high‐voltage EDLCs due to their superior voltage window, electrochemical performance, and predominant safety aspects. Mindful of this, the current report demonstrates the electrochemical performance of new nanoporous carbon electrodes derived from waste dry leaves of Swietenia macrophylla with a high specific surface area (SSA) (1834 m2 g−1) in polymer–gel, WIS, and ionic liquids‐based electrolytes. Symmetric EDLC devices are fabricated using polymer gel solid‐state (PVA–Na2SO4), ionic liquids (EMIMBF4), and WIS (21 m LiTFSI) electrolytes with the electrochemical stability windows of (ESW) 2, 2.5, and 2 V, respectively. The assembled devices with Na2SO4/PVA, EMIMBF4, and 21 m LiTFSI (WIS) electrolytes‐based devices exhibit high energy densities of 40, 31, and 25 Wh kg−1 at 0.5 A g−1 and good output power delivery of 5, 6.23, and 3 kW kg−1 at 5 A g−1 with better cyclability features. Self‐discharging studies and systematic evaluation of high‐voltage EDLCs offer a sustainable method to develop high‐performance aqueous and diverse electrolyte‐based supercapacitors. [ABSTRACT FROM AUTHOR]

The document is the contents list for an issue of the journal Chemical Communications. It includes the titles and authors of various articles that will be featured in the issue. Some of the topics covered include PGM-free single atom catalysts, challenges and advances in MOF-based gas separation membranes, and the synthesis and stability of a Ti-DOTA complex. The journal is published by The Royal Society of Chemistry and is dedicated to sustainable chemistry and new solutions. [Extracted from the article]

In this work, a SiO2 doped polyvinyl alcohol/polyethylene glycol (PVA/PEG) gel polymer electrolyte (PVA/PEG-SiO2) was constructed via an ice-crystal template for zinc-ion batteries. The SiO2 and the three-dimensional porous skeleton make it have excellent ionic conductivity and mechanical strength, and inhibit the growth of dendrites. The assembled ZIBs exhibit excellent rate performance and cycle stability, making it a promising electrolyte membrane candidate for flexible wearable electronics. [ABSTRACT FROM AUTHOR]

In situ formation of gel polymer electrolytes (GPE) has been a promising candidate to address individual limitations of liquid/solid electrolytes and interfacial stability. However, the controllable conversion of liquid electrolyte (LE) precursor to GPE remains a great challenge with lower lithium‐ion transport, which is far from the demand for fast‐charging properties. Herein, a strategy of gradient polymerization of forming GPE is pioneered, stabilizing the electrolyte/electrode interface with an accelerated Li+ migration feature. As demonstrated by theoretical simulations and visualization experiment results, the formation mechanism of GPE via a partial inhibitory mechanism of Lithium nitrate (LiNO3) to control the solvent polymerization is comprehensively investigated, exhibiting the preferential interaction between nitrate anion (NO3−) and the Lewis acidic site in lithium bis(fluorosulfonyl)imide (LiFSI). Consequently, a stable amorphous GPE with high Li+ conductivity (5.10 mS cm−1) and an inorganic solid electrolyte interphase (SEI)‐dominate layer derived from spectroscopical measurements are achieved on the graphite electrode surface. The as‐prepared lithium iron phosphate (LFP)||graphite pouch cell stabilizes the capacity of 109.80 mAh g−1 (capacity retention: 80.02%) after 715 cycles at 5 C/1 C (charge/discharge), corresponding to the energy density of 277.64 Wh kg−1. This work provides a facile but practical approach to designing a highly stable GPE for fast‐charging lithium‐ion batteries. [ABSTRACT FROM AUTHOR]

Considerable research has been conducted on single-ion conductive polymeric electrolytes with high lithium ion transference numbers. However, low ionic conductivity is a long-standing challenge for lithium metal batteries, hindering the development of extending their cycle life. In this study, we synthesized a novel fluorine-containing single-ion polymeric electrolyte, LiP(VDF-co-MAF)BB (Polyvinylidene fluoride trifluoromethyl acrylate lithium borate polymer; subsequently referred to as PPMBB), exhibiting a room temperature conductivity of 1.03 × 10−3 S/cm. This electrolyte demonstrates a high lithium ion transference number of 0.7901 and an extended electrochemical stability window of 5.5 V. Under a 2 C discharge rate, it manifests a remarkable discharge specific capacity of 146.8 mAh/g. Moreover, even after 364 cycles, the capacity retention remains at 76%. The single-ion polymeric gel electrolyte designed in this work provides a promising strategy for the prolonged cycling performance of lithium metal batteries. [ABSTRACT FROM AUTHOR]

In this work, Co3O4 spinel is synthesized and exposed as cathode material because of its high stability in alkaline electrolytes, high working voltage window in full cell (vs. Zn) > 1.75 V, high specific capacity (446 mAh g−1), having a high theoretical energy density of 516 Wh kg−1, and good electrochemical stability. Here, the Co3O4 sample was synthesized using a simple co-precipitation process followed by calcination. X-ray diffraction was used to confirm the structure and phase purity of the samples. The surface morphology of the sample was examined using FESEM and HR-TEM analysis. The oxidation state of Co in the sample was evaluated using XPS analysis. The Zn||PVA-KOH||Co3O4 electrochemical cell was fabricated, and the electrochemical performance was investigated. Here, we used gel polymer electrolyte to demonstrate the practical feasibility of the flexible Zn||Co3O4 cell. Polyvinyl alcohol (PVA) gives excellent chemical stability and electrochemical inertness, is easy to fabricate, and is non-toxicity; in this work, it is used as a host polymer, and potassium hydroxide (KOH) is used as an ion source in the gel electrolyte medium. Here, PVA is used as a polymer host and separator to separate the anode and cathode in the full cell fabrication. The hydrogel-based pouch-type full cell retained good capacity over 1000 cycles with the maximum tested cell capacity of 10 mAh cm−2 at 2 mA cm−2. The cell showed above > 95 capacity retention even at 1000 cycles, which indicates that the Co3O4 can be used as a potential cathode in 1.6 V aqueous Zn cells. [ABSTRACT FROM AUTHOR]

Comprehensive Summary Polycatenane gels have attracted extensive attention due to their high degree of freedom and mobility. However, the syntheses of poly[2]catenane gels reported to date all rely on the polymer as the backbone. Herein, we prepared poly[2]catenane gels based on entirely sequential assembly of small molecules. Monomer M1 with two unclosed rings was first prepared, which self‐assembled to form supramolecular polymers (SPs) via hydrogen bonding and π‐π interactions. Upon adding small molecule monomers M2 and M3 with aldehyde groups, ring closing of SPs occurred because the amino groups in the SPs reacted with M2 to form imine bonds. In addition, M3, which had twice the number of aldehyde groups as M2, enabled SPs to ring‐close, causing the proceeding of crosslinking process at the same time. Thus linear SPs were transformed into poly[2]catenane gel networks. Due to the presence of hydrogen bonds in the poly[2]catenane gel, the gel also possessed stimulus responsiveness and self‐healing properties. [ABSTRACT FROM AUTHOR]

High‐voltage lithium‐metal batteries (LMBs) are promising for energy storage applications but suffer from poor electrochemical window of solid polymer electrolytes (SPEs), which are difficult to achieve via a single polymeric functionality. Herein, a hybrid Si/F‐based polymeric 3D network is reported bearing polysiloxane backbone with fluorinated pendants to tune the highest occupied molecular orbital (HOMO)/the lowest unoccupied molecular orbital LUMO energies, thermodynamically expanding intrinsic electrochemical window of solid polymer electrolyte (SPE). Meanwhile, the hybrid Si/F functionalities with high fluorine abundance is identified to furnish dual interfacial kinetic stability at both anode and cathode interfaces with stabilized solid electrolyte interface (SEI) and cathode electrolyte interface (CEI), respectively. As a result, stable cycling in solid‐state high‐voltage LMBs is achieved up to an ultrahigh operating voltage of 4.9 V. Furthermore, it shows that in situ blending the Si/F SPE with eutectic electrolytes (EE) to form a non‐flammable gel polymer electrolyte can mitigate parasitic reactions of EE against metallic Li anode and achieve highly reversible charge–discharge cycling from 4.2 to 4.8 V at 25 °C. [ABSTRACT FROM AUTHOR]

Structurally colored objects with 3D geometries are intriguing in optical devices and visual sensors, but their preparation is bottlenecked by complicated procedures and limited material choices. Herein, a facile supramolecular 3D printing strategy is proposed via direct ink writing (DIW) supramolecular colloidal inks (SCIs) consisting of polymers and colloids based on supramolecular interactions to construct healable and recyclable structurally colored objects. Optimized supramolecular interactions balance the rheological requirements for DIW and the high particle volume fraction for the one‐step and immediate generation of structural color. The shear‐thinning and thixotropy features of the SCIs, characterized by a two‐order‐of‐magnitude decrease in viscosity during the printing process and 50% storage modulus recovery thereafter, ensure the reversible solid–liquid transition during the extrusion and deposition process. The short‐range ordered arrangements of colloids within the matrix give rise to angle‐independent structural color. Moreover, 3D structurally colored objects from the SCIs are healable and, more importantly, can be closed‐looped recycled thanks to the reversibility of supramolecular interactions. Leveraging optimized supramolecular interactions, various SCIs with a wide range of material choices meeting the DIW process are extended to construct 3D structurally colored objects directly. This study paves the way for constructing advanced 3D materials with a supramolecular strategy. [ABSTRACT FROM AUTHOR]

Gels with excellent ionic conductivity and resilience to temperature extremes are sought in practical applications due to their potential for building flexible and wearable soft electronics. In this work, highly conductive eutectogels are fabricated by one‐step polymerization of (3‐acrylamidopropyl) trimethyl ammonium chloride in deep eutectic solvents (DESs). Owing to the ion‐conductive polymer networks facilitating ion conduction, these eutectogels exhibit a significant enhancement in ionic conductivity (27.1 mS cm−1), demonstrating an order of magnitude higher than that of pure DES. Furthermore, due to several unique properties of DES, these eutectogels exhibit excellent stretchability (>1000%), good adhesion, as well as nonflammability performance over a wide temperature range (−40 to 100°C). Moreover, the strain sensor based on the eutectogel shows a highly sensitive response (gauge factor = 6.92) to a broad strain range (from 450% to 550%), enabling the accurate and reliable detection of various human movements. Additionally, our findings reveal that the eutectogel‐based sensor displays a comparable pattern of response curves with negligible signal deterioration, even at extreme temperatures of −20 and 60°C. The results of this work will promote novel applications in the construction of flexible and safe devices. [ABSTRACT FROM AUTHOR]

Sodium metal batteries (SMBs) can be developed on a large scale to achieve low‐cost and high‐capacity energy storage systems. Gel polymer electrolyte (GPE) can relieve volatilization of liquid electrolyte, adapt to volume changes in electrodes, and better satisfy the requirements of long‐term SMBs. Herein, a dense polyurethane‐based GPE modified with polyacrylonitrile is synthesized by rapidly swelling two‐component polyurethane/polyacrylonitrile electrospun fiber film. Compared to traditional porous GPEs obtained by swelling porous matrixes, the fiber film provides uniform high Na+ flux inside GPE due to its partial solubility property and ability to dissociate salts. Therefore, it can reduce the polarization effect and induce uniform metal deposition under high current in conjunction with its constructed hybrid N/F‐containing solid electrolyte interface (SEI) that possesses low ionic diffusion barrier. The study demonstrates that GPE has an ionic conductivity of 1.816 mS cm−1 at 20 °C and an ion transference number of 0.53. The full battery (NVP/GPE/Na) assembled with this GPE and Na3V2(PO4)3 (NVP) cathode shows 90.8% capacity retention rate after 1000 cycles at 10 C. Considering the convenient preparation and outstanding electrochemical performances of the obtained GPE, it can also be matched with other electrodes in the future to expand the application of sodium‐based batteries. [ABSTRACT FROM AUTHOR]

This work focuses on studying the effect of Sodium Dodecyl Sulphate (SDS) at its critical micelle concentration (CMC) on the performance of ion conducting gel polymer electrolytes (GPEs) for supercapacitors. By incorporating SDS at its CMC, the morphology of GPE were altered, leading to improved ion transport properties. Additionally, SDS influenced the electrode-electrolyte interface, resulting in modifications to the charge storage mechanisms and capacitance values. The GPE exhibited a high ionic conductivity of 5.6 mS/cm. The resulting supercapacitor demonstrated exceptional performance with respect to the blank supercapacitor, including high specific capacitance, energy density, as well as low self-discharge characteristics. The specific capacitance of the supercapacitor was measured to be 18.01 Fg-1, while the energy density reached 0.362 Wh/kg. Furthermore, the supercapacitor exhibited a power density of 2.00 kW/kg. The electrolyte was analysed using impedance studies to study the effects of SDS micelles on the properties of the electrolyte film. The GPE was sandwiched between two Laser Induced Graphene (LIG) electrodes prepared from (Polyimide) PI Sheets. Cyclic Voltammetry (CV), Galvanostatic Charge-discharge (GCD), and Electrochemical Impedance Spectroscopy (EIS) was done to study the electrochemical characteristics of the supercapacitors. [Display omitted] • SDS micelles was used to improve the ion-transport of the PVA-Ammonium Acetate-based Gel-polymer electrolyte. • Presence of micelles showed an improvement in conductivity and dielectric properties. • Micelle modified electrolyte shows significant reduction in charge-transfer resistance and solution resistance. • Micelle modified electrolyte reduced self-discharge, retaining 35% of its initial voltage. [ABSTRACT FROM AUTHOR]

Self‐oscillating gel systems exhibiting an expanded operating temperature and accompanying functional adaptability are showcased. The developed system contains nonthermoresponsive main‐monomers, such as N,N‐dimethylacrylamide (DMAAm) or 2‐acrylamido‐2‐methylpropane sulfonic acid (AMPS) or acrylamide (AAm) or 3‐(methacryloylamino)propyl trimethylammonium chloride (MAPTAC). The gels volumetrically self‐oscillate within the range of the conventional (20.0 °C) and extended (27.0 and 36.5 °C) temperatures. Moreover, the gels successfully adapt to the environmental changes; they beat faster and smaller as the temperature increases. The period and amplitude are also controlled by tuning the amount of main‐monomers and N‐(3‐aminopropyl) acrylamide. Furthermore, the record amplitude in the bulk gel system consisting of polymer strand and cross‐linker at 36.5 °C is achieved (≈10.8%). The study shows new self‐oscillation systems composed of unprecedented combinations of materials, giving the community a robust material‐based insight for developing more life‐like autonomous biomimetic soft robots with various operating temperatures and beyond. [ABSTRACT FROM AUTHOR]

High sulfur content polymeric materials, known for their intriguing properties such as high refractive indices and high electrochemical capacities, have garnered significant interest in recent years for their applications in optics, antifouling surfaces, triboelectrics, and electrochemistry. Despite the high interest, most high sulfur‐content polymers reported to date are either bulk materials or thin films, and there is a general lack of research into sulfur‐rich polymer colloids. Water‐dispersed, sulfur‐rich particles are anticipated to broaden the range of applications for sulfur‐containing materials. In this study, the preparation and size control parameters are presented of an aqueous dispersion of sulfur‐rich polymers with the sulfur content of dispersed particles exceeding 75 wt%. Employing polymeric stabilizers with varying hydrophilic‐lipophilic balance (HLB), along with changing the rank of inorganic polysulfides, allow for the control of particle size in the range of 360 nm – 1.8 µm. The sulfur‐rich colloid demonstrates antioxidant properties in water, demonstrating the potential for the use of sulfur‐rich polymeric materials readily removable, heterogeneous radical scavengers. [ABSTRACT FROM AUTHOR]

Temperature dependence of ionic conductivity of three different compositions of the Mg(BH4)2:polyethylene oxide (PEO):propylene carbonate (PC) polymer gel electrolyte with Mg(BH4)2:PEO molar ratios of 1:8, 1:10, and 1:12 was studied. The composition with Mg(BH4)2:PEO = 1:10 exhibited the highest ionic conductivity of 7.60 × 10−6 S cm−1 at 30 °C. The effect of TiO2 nanofiller on ionic conductivity enhancement was studied for Mg(BH4)2:PEO:PC:TiO2 polymer gel electrolyte by varying the TiO2 weight ratio from 0 to 12.5 wt.%. The highest ionic conductivity of 17.95 × 10−6 S cm−1 at 30 °C was exhibited by the electrolyte composition with 10 wt% of TiO2 nanofiller. The optimized electrolytes had a Mg++ cationic transference number of 0.22 for the filler free electrolyte and 0.30 for the TiO2 10wt% filler incorporated electrolyte. Both electrolytes had negligible electronic conductivity. A more than two-fold increase in the ionic conductivity and a 30% increase in Mg++ ion transference number can be attributed to the nanofiller effect caused by TiO2. This preliminary study shows the possibility of developing this PEO-based polymer gel electrolyte to be used in rechargeable Mg ion batteries. [ABSTRACT FROM AUTHOR]

Gel‐state polymer electrolytes with superior mechanical properties, self‐healing abilities and high Li+ transference numbers can be obtained by in situ polymerization of monomers with hydrogen‐bonding moieties. However, it is overlooked that the active hydrogen atoms in hydrogen‐bond donors experience displacement reactions with lithium metal in lithium metal batteries (LMBs), leading to corrosion of the lithium metal. Herein, it is discovered that the addition of hydrogen‐bond acceptors to hydrogen‐bond‐rich gel‐state electrolytes modulates the chemical activity of the active hydrogen atoms via the formation of hydrogen‐bonded intermolecular interactions. The characterizations reveal that the added hydrogen‐bond acceptors encapsulate the active hydrogen atoms to suppress the interfacial chemical corrosions of lithium metals, thereby enhancing the chemical stability of the polymer structure and interphase. With the employment of this strategy, a 1.1 Ah LiNi0.8Co0.1Mn0.1O2/Li metal pouch cell achieves stable cycling with 96.3 % capacity retention at 100 cycles. This new approach indicates a feasible path for achieving in situ polymerization of highly stable gel‐state‐based LMBs. [ABSTRACT FROM AUTHOR]

The World Health Organization (WHO) estimates that microbiologically contaminated drinking water is estimated to cause 485,000 diarrheal deaths each year. Household water treatment is a low-cost method for reducing the pathogen load in drinking water to decrease instances of diarrhea and sometimes death. This study developed and evaluated a new silver and copper water treatment product that meets WHO one-star performance criteria for household water treatment without using electricity: the MadiDrop+Cu. First, we tested different configurations of a copper mesh and a copper screen with the MadiDrop to evaluate the effects of their proximity to one another on copper and silver concentrations in water. Wrapping the copper mesh around the MadiDrop decreased silver concentrations in water compared with the MadiDrop alone. Folding the copper screen into smaller dimensions decreased the copper concentrations in water compared with the copper screen unfolded. The MadiDrop and copper screen, coined MadiDrop+Cu , provided an average of 125–415 μg/L copper and 4–21 μg/L silver daily for 150 days of use. When tested individually and in combination against E. coli, MadiDrop+Cu removed the most bacteria together rather than separately after 8 h. A previous study found a prototypic chlorinated polymer gel removed more E. coli with the MadiDrop than either intervention alone after 8 h. This study tested the viral (MS2 Bacteriophage) disinfection from the chlorinated polymer and MadiDrop+Cu by themselves and in combination with one another. The MadiDrop alone removed <1 log (90%) of viruses, whereas MadiDrop+Cu removed >3 log (99.9%) after 24 h. The greatest viral disinfection occurred when the MadiDrop+Cu and chlorine-charged polymer gel were used together, removing >4 log (99.99%) after 24 h. Practical Applications: Low-cost and simple household water treatment products can be used in underresourced settings to prevent waterborne disease. This study designed and tested a novel approach to low-cost water treatment: combining a silver-embedded ceramic tablet with a high specific-surface-area copper screen and a chlorine-charged polymer gel. MadiDrop+Cu was found to consistently release sufficient levels of silver and copper over 150 days of use. The MadiDrop alone killed less than 90% of viruses, whereas the MadiDrop+Cu killed over 99.9% of viruses after 24 h. The MadiDrop, copper screen, and the chlorine-charged polymer gel killed over 99.99% of viruses after 24 h. Although a 24 h wait time is not ideal for emergency settings, the findings suggest that this novel approach to combining silver, copper, and chlorine without electricity is a promising method for a low-cost, household water treatment. [ABSTRACT FROM AUTHOR]

This study uses fly-ash-based superplasticized geopolymer by adding a naphthalene-centered superplasticizer to the geopolymerized soil. Alkali-binder ratios and alkali-activator ratios are varied simultaneously with a molarity of 10M. The optimum dosages of binder, geopolymer, and superplasticized geopolymer are found from unconfined compression tests. California Bearing Ratio (CBR), pH, consolidation, water-holding capacity, and microstructure tests were performed on optimum dosages. The clayey soil's undrained shear strength and CBR value increased as the geopolymer was superplasticized. The 28-day undrained shear strength of geopolymerized clay was around 300 kPa, attained within three days of the curing period with superplasticized geopolymer. This is because adding a superplasticizer increases the polymerization reaction rate and improves the geopolymer's performance. The maximum undrained shear strength was attained within seven days of the curing period for both cases. The undrained shear strength after a curing period of 7, 14, and 28 days for geopolymer and superplasticized geopolymer was found to be almost the same value, which shows that after seven days, curing has little role in strength improvement. The hydraulic conductivity and coefficient of consolidation of geopolymerized soil increased with the addition of superplasticizer due to the reduction in fine particles and plasticity of the residual soil. Microstructural studies using scanning electron microscope and x-ray diffraction techniques showed an interaction between soil, geopolymer, and superplasticizer, thus confirming the formation of geopolymer gel and increased polymerization rate with the superplasticizer. [ABSTRACT FROM AUTHOR]

Polymer gel has been accepted as a useful tool for solving many sealing operations such as fluid loss control, enhanced oil recovery, water and gas shutoff, wellbore integrity, and well stimulation in the upstream of petroleum industry. In a previous study, we used acrylamide (AM), N,N'-Methylenebisacrylamide (MBA), xanthan (XC) and chromium acetate (Cr3+) to obtain ultra-high strength gel (USGel). Some interesting phenomena, such as the more than 10 times increase in gel strength by 0.05% Cr3+ and the counter-conventional decrease in gel strength by inorganic particles such as layered silicate materials (LSM), silicon dioxide nanoparticles (SiO2) and laponite (RDS), have not been well explained. In this paper, the gelation kinetics and mechanism of USGel were investigated mainly by bottle, DSC, infrared spectroscopy, and environmental scanning electron microscopy (ESEM) experiments, which explained that Cr3+ significantly increased the gel strength of USGel, while inorganic particles had a negative effect on the gel strength. The experimental results showed that Cr3+ preferentially cross-linked AM and XC than MBA, and the gelation rates of Cr3+-XC and Cr3+-AM were 107% and 92.9% faster than AM-MBA, respectively. It is speculated that the triple network structure and physical entanglement formed by AM-MBA, XC-Cr3+, and AM-Cr3+ are the main reasons for significant improvement of gel strength by Cr3+, and the cross-linking competition between LSM and Cr3+ and reduction of entanglement number are the main reasons for the significant reduction of gel strength by LSM. This paper provides new insights into the preparation of ultra-high strength gels and the usage of inorganic particles. [ABSTRACT FROM AUTHOR]

Crosslinked polymer films, formed via sol–gel and UV photocrosslinking, serve as gel polymer electrolytes (GPEs) in lithium‐ion batteries. Combining polyurethane acrylate (PUA), polyurethane methacrylate (PUMA), pentaerythritol tetrakis (3‐mercaptopropionate) (PETMP), and 3‐mercaptopropyl trimetoxysilane (MPTMS) yields flexible membranes, enhancing stability and liquid electrolyte compatibility. The resulting GPE displays higher ionic conductivity (1.46 × 10−3 S cm−1) than Celgrad2500, with PUA‐PUMA's hydrophilicity and PETMP's SH groups preventing leakage. GPPF1, the developed GPE, offers improved ionic conductivity, a stable electrochemical window up to 3.8 V, and heightened safety for versatile energy storage systems. [ABSTRACT FROM AUTHOR]

In order to solve the problem of poor stability of HPAM (partially hydrolyzed polyacrylamide) gel as a plugging agent at 150 °C, this paper investigates the preparation of a polymer gel strengthened with nano-SiO2, exhibiting good thermal stability, using a low-cost, low-hydrolysis anionic polymer. The experimental results indicated that when the gel was prepared with 1 wt% HPAM, 1 wt% water-soluble phenolic resin (WSPR) as a crosslinker, and 1 wt% nano-SiO2 as a stabilizer, the dehydration rate of the gel was less than 5 wt% after 180 days of aging at 150 °C. In order to identify the stability mechanism of nano-SiO2-strengthened polymer gel, we conducted rheological tests, Cryo-SEM analysis, Fourier transform infrared (FTIR) spectroscopy, and solid-state nuclear magnetic resonance (NMR) analysis on the polymer gel before and after adding nanoparticles. The methods described in the study demonstrate the excellent long-term thermal stability of the polymer gel strengthened with nano-SiO2 from both chemical bonding and microscopic perspectives. The results of rheological experiments indicated that the addition of nanoparticles improved the yield stress and long-term thermal stability of the gel. The scanning electron microscope (SEM) microstructure analysis confirmed that the addition of nanoparticles resulted in high-density cavities between the microscopic network structures of the gel. This facilitated the trapping of a significant amount of free water and the formation of a stable spatial mechanical support structure, ultimately enhancing the macro-mechanical strength of the gel. Additionally, FTIR and NMR experiments demonstrated that the nanoparticles effectively inhibited the hydrolysis of amide groups to carboxylate, thereby significantly preventing the high-temperature degradation of the gel and maintaining its strength after prolonged aging. [ABSTRACT FROM AUTHOR]

Hypothesis Long-acting formulations such as microparticles, injectable depots and implantable devices can realize spatiotemporally controlled delivery of protein drugs to extend their therapeutic in vivo half-lives. To efficiently encapsulate the protein drugs into such drug delivery systems, (sub)micron-sized protein particles are needed. The formation of micronized supraproteins can be induced through the synergistic combination of attractive depletion forces and freezing. The size of the supraproteins can be fine-tuned from submicron to several microns by adjusting the ice crystallization rate through the freeze-quench depth, which is set by the target temperature. Methods Supraprotein micron structures were prepared from protein solutions under various conditions in the presence and absence of nonadsorbing polyethylene glycol. Scanning electron microscopy and dynamic light scattering were employed to determine the sizes of the supraproteins and real-time total internal reflection fluorescent microscopy was used to follow the supraprotein formation during freezing. The protein secondary structure was measured before and after micronization by circular dichroism. A phase diagram of a protein–polyethylene glycol mixture was theoretically predicted to investigate whether the depletion interaction can elucidate the phase behavior. Findings Micronized protein supraparticles could be prepared in a controlled manner by rapid freeze-drying of aqueous mixtures of bovine serum albumin, horseradish peroxidase and lysozyme mixed with polyethylene glycol. Upon freezing, the temperature quench initiates a phase separation process which is reminiscent of spinodal decomposition. This demixing is subsequently arrested during droplet phase separation to form protein-rich microstructures. The final size of the generated protein microparticles is determined by a competition between phase separation and cooling rate, which can be controlled by target temperature. The experimental phase diagram of the aqueous protein–polyethylene glycol dispersion aligns with predictions from depletion theory for charged colloids and nonadsorbing polymers. Supraproteins of varying sizes emerge through the synergistic interplay of attractive depletion forces and freezing. This is demonstrated through aqueous protein-polyethylene glycol dispersions across different target temperatures. • Supraproteins can be prepared via freezing protein–polyethylene glycol in water dispersions. • The size of these supraproteins can be tuned via the depletion concentration and cooling rate. • Initial composition of protein–polyethylene glycol mixtures affects supraprotein formation. • The phase diagram of charged proteins and polyethylene glycol is quantified using depletion theory. • Proteins preserve their secondary structure during supraprotein formation process. [ABSTRACT FROM AUTHOR]