Ionic Loading Research Articles

Enabling room temperature solid-state lithium batteries by blends of copolymers and ionic liquid electrolytes

High lithium-concentration phosphonium ionic liquids electrolytes have shown outstanding properties even overcoming ammonium derivatives in terms of viscosity and transport properties. Consequently, they have been also combined with fluorinated polymers, such as poly(vinylidene fluoride) (PVDF) or poly(ionic liquids), for solid-state batteries with satisfying performance at 50 °C. The aim of this work is to develop highly lithium conducting solid-state electrolyte (≥0.1 mS cm−1) at room temperature but maintaining solid-state properties. For this, polymer electrolytes based on ISOBAM alternating copolymer (isobutylene and maleic anhydride) and ionic liquid (P111i4FSI) were developed. The composition-dependent behavior of the solid electrolytes was studied in terms of electrochemical impedance spectroscopy (EIS), reaching σLi+ of 0.52 mS cm−1; differential scanning calorimetry (DSC) and Fourier-transform infrared spectroscopy (FTIR) under different ionic liquid electrolyte loadings and salt concentration. The polymer electrolytes presented a solid-like behavior in the range of 25 to 90 °C with a storage modulus of 2.3·104 Pa. Finally, the best free-standing membrane electrolytes were tested and compared electrochemically in lithium symmetrical cells and lithium iron phosphate full cells exhibiting an excellent cycling at room temperature.

Construction of trifloaluminate ionic liquid catalyst on the silica surface dedicated for continuous flow Diels-Alder synthesis

Supported ionic liquid phases (SILP) are efficiently use for the construction of highly active, heterogeneous and recyclable catalysts. In this study, three strategies towards chemical immobilization of trifloaluminate ionic liquid catalyst into microporous/mesoporous silica support were investigated. The order of silica surface modification with trifloaluminate ILs components had crucial influence on the catalytic activity and stability which was tested in the model Diels-Alder reaction between isoprene and maleic anhydride in acetonitrile at room temperature. The best catalytic performance (maleic anhydride conversion > 97% in ten reaction cycles) was achieved for catalyst created through the synthesis of trifloaluminate ionic liquid in the first step with further bounding to the silica surface using 25 wt% of ionic liquid loading. The effective transformation of the Diels-Alder reaction to continuous flow synthesis led to 97% maleic anhydride conversion over 432 h with a TOF of 104.3 h−1 and significantly improved process sustainability.

Solid Polymer Electrolytes with Enhanced Electrochemical Stability for High‐Capacity Aluminum Batteries

AbstractChloroaluminate ionic liquids are commonly used electrolytes in rechargeable aluminum batteries due to their ability to reversibly electrodeposit aluminum at room temperature. Progress in aluminum batteries is currently hindered by the limited electrochemical stability, corrosivity, and moisture sensitivity of these ionic liquids. Here, a solid polymer electrolyte based on 1‐ethyl‐3‐methylimidazolium chloride‐aluminum chloride, polyethylene oxide, and fumed silica is developed, exhibiting increased electrochemical stability over the ionic liquid while maintaining a high ionic conductivity of ≈13 mS cm−1. In aluminum–graphite cells, the solid polymer electrolytes enable charging to 2.8 V, achieving a maximum specific capacity of 194 mA h g−1 at 66 mA g−1. Long‐term cycling at 2.7 V showed a reversible capacity of 123 mA h g−1 at 360 mA g−1 and 98.4% coulombic efficiency after 1000 cycles. Solid‐state nuclear magnetic resonance spectroscopy measurements reveal the formation of five‐coordinate aluminum species that crosslink the polymer network to enable a high ionic liquid loading in the solid electrolyte. This study provides new insights into the molecular‐level design and understanding of polymer electrolytes for high‐capacity aluminum batteries with extended potential limits.

Trifloaluminate Ionic Liquids Supported UIO‐67 as Lewis Acidic Catalyst for Excellent Synthesis of Alkyl Levulinates

AbstractHerein, levulinate acid esters (LAEs) were efficiently synthesized from the α‐angelica lactone (α‐AL) esterification with trifloaluminate ionic liquids supported UIO‐67 MOF as Lewis acidic catalyst. A series of UIO‐67 catalysts with varied trifloaluminate ionic liquids loading were prepared via the post‐modification method and exhibited excellent catalytic activity for α‐AL esterification. Remarkable α‐AL conversion (100 %) and LAEs selectivity (>99 %) were achieved by UIO‐67 catalysts (0.2 mol %) with 12.4 %, trifloaluminate ionic liquids loading (UIO‐67‐TFA) at 70 °C and 90 min. The UIO‐67‐TFA catalyst can be reused at least 5 cycles without significant loss of catalytic activity. The UIO‐67‐TFA catalysts were fully characterized by XRD, SEM, XPS, TGA, IR, N2 physisorption, etc. The results indicated that the well‐distributed active trifloaluminate Lewis acid catalytic sites, high BET surface area, and good thermal stability could contribute to its excellent catalytic activity.

Chemical composition of fogwater collected at four sites in North- and Mount-Lebanon during 2021

A field campaign is established at four sites in North-Lebanon (Akkar district) and Mount-Lebanon (Keserwan district) for the first time between February and June 2021 using the Caltech Active Strand Cloud Collector (CASCC). Overall, 14 fog events are sampled, of which 5 samples from Fnaideq, 5 samples from Beit Younes, 1 sample from Qamouaa, and 4 samples from Bzomar. Their mean liquid water content (LWC) varies between 0.023 and 0.045 g m−3, their mean conductivity (K) varies between 53.3 and 2210 μS cm−1, and their pH varies between 6.5 and 7.8. The dissolved organic carbon (DOC) varies between 7.4 and 82.6 ppm. DOC shows a good correlation with magnesium and chloride, and no relationship with the liquid water content (LWC). The total average ionic concentrations (TIC) in Fnaideq, Qamouaa, Beit Younes, and Bzomar are respectively 3106.9, 4112.2, 4972.4, and 5969.1 μEq L−1. TIC shows a negative correlation with LWC (r2 = 0.7), suggesting that an increase in the LWC with dilute the solute concentration. The fog water in Lebanon is characterized by high concentrations of Ca2+ (35% of the measured TIC), Na+ (20%), Cl− (12%), NH4+ (11%), and Mg2+ (11%). The contribution of the acidic ions (SO42− and NO3−) from industrial and vehicular sources is minimum (respectively of 3% and 1%). NH4+, originating from the scavenging of gaseous ammonia and particulate ammonium nitrate and sulfate and from agricultural activities, and Ca2+‏, originating from the scavenging of coarse particles, act as acid neutralizers and are the main cause for the relatively basic pH of fogs in Lebanon. The contribution of Ca2+ and Mg2+ to sea-salt is found to be negligible, whereas the contribution of SO42− to sea salt is higher. Zn and Ni are the most two abundant heavy metals at all sampling sites. Their concentrations vary respectively between 137.6 and 349.7 μg L−1 (mean of 211.8 μg L−1) and between 38.2 and 585.5 μg L−1 (mean of 197.6 μg L−1). They account together for an average of 58% of the total elemental concentration. The high enrichment factors (higher than 100) for Ni, Cu, Zn, Hg, and Cd suggest significant anthropogenic contamination at the sampling sites. The ionic sources are also determined by the Principal Component Analysis (PCA). Two principal components (PCs) that account together for 62% of the total variance are identified by PCA. High ionic loadings are observed indicating a well-mixed mixture of local anthropogenic sources (factories, motor vehicle emissions, sea transportation, agriculture, combustion, civil construction, etc.) and some natural sources (sea and crust/soil).

Highly stable Lewis acidic trifloaluminate ionic liquid supported on silica and metallosilicates as an efficient catalyst for continuous flow aminolysis of epoxides

In this work heterogeneous catalysts based on hybrid materials consisted of calcium and/or magnesium silicates and modern task-specific ionic liquids (supported ionic liquid phase material) dedicated particularly for continuous flow synthesis of fine chemicals with liquid reagents were designed. Pure SiO2 (as a reference sample), as well as magnesium (MgO-SiO2) or calcium (CaO-SiO2) silicates were used as supports for Lewis acidic trifloaluminate ionic liquids immobilized via chemical bound. The lowest ionic liquid loading was determined for SiO2 (15.58 wt%) and the highest for CaO-SiO2 (23.70 wt%). Resulted catalysts were used for the optimization of process parameters of the synthesis of β-amino alcohols in batch reactor (molar ratio aniline: styrene oxide 1.1:1; 1 mol% of catalyst, 60 °C). Not only the most active (conversion of styrene oxide 100.0% and selectivity to main product 98.7%) but also stable in 3 cycles of the process was the catalyst based on MgO-SiO2. The activity of poorly recyclable precursor of ionic liquid used as an active phase Al(OTf)3 was also lower (conversion 87.3% and selectivity 94.6%). Substrate scope confirmed the versatility of this method. The key achievement of the research was the confirmation of activity and stability of the most active catalyst in batch process for the aminolysis of epoxide in the presence of heterogeneous catalyst based on MgO-SiO2 in flow system through 72 h (conversion 81.1%, selectivity 95.9%). The proof of concept for the design of this catalytic system for production of selected fine chemicals is shown in this study.

Design of healable, porous polyurethane with large ionic liquids loading amounts towards ultra-durable pressure sensor

Flexible intelligent sensors have got booming development over the past decades, yet, it is still a huge challenge to construct advanced sensors with long service life and superb durability. Herein, a novel porous capacitance pressure sensor with ultra-durability via sugar template method was prepared successfully by impregnating non-volatile, highly conductive ionic liquids (ILs) into polyurethane (PU-DBTDA5) matrix. As a consequence of the rich hydrogen bonding networks and dynamic hindered urea bond in the polymer chain, the as-prepared PU-DBTDA5 matrix shows excellent self-healing ability (99 %). The ionic liquid-soluble polyethylene glycol (PEG1000) serving as soft segment endows PU-DBTDA5 with ultra-absorption ability of ILs (absorbing ILs over three times to its own weight within 5 min). The pressure sensor with porous structure shows outstanding anti-fatigue ability as well as good sensitivity (S1 = 0.82 kPa−1, S2 = 1.04 kPa−1), and it can even monitor tiny strain as low as 0.5 %. More importantly, due to the well combination of the PU-DBTDA5 with excellent self-healing ability and the non-volatile ionic liquids, not only the healed sensor, but the sensor stored at room environment over 100 days both exhibit stable electronic signals similar to that of freshly-prepared foam sensor in 3000 uninterrupted compression tests, being strong evidence of its ultra-durability.

Valorization of Hemp-Based Packaging Waste with One-Pot Ionic Liquid Technology.

The range of applications for industrial hemp has consistently increased in various sectors over the years. For example, hemp hurd can be used as a resource to produce biodegradable packaging materials when incorporated into a fungal mycelium composite, a process that has been commercialized. Although these packaging materials can be composted after usage, they may present an opportunity for valorization in a biorefinery setting. Here, we demonstrate the potential of using this type of discarded packaging composite as a feedstock for biofuel production. A one-pot ionic liquid-based biomass deconstruction and conversion process was implemented, and the results from the packaging material were compared with those obtained from untreated hemp hurd. At a 120 °C reaction temperature, 7.5% ionic liquid loading, and 2 h reaction time, the packaging materials showed a higher lignocellulosic sugar yield and sugar concentrations than hemp hurd. Hydrolysates prepared from packaging materials also promoted production of higher titers (1400 mg/L) of the jet-fuel precursor bisabolene when used to cultivate an engineered strain of the yeast Rhodosporidium toruloides. Box-Behnken experiments revealed that pretreatment parameters affected the hemp hurd and packaging materials differently, evidencing different degrees of recalcitrance. This study demonstrated that a hemp hurd-based packaging material can be valorized a second time once it reaches the end of its primary use by supplying it as a feedstock to produce biofuels.

Lewis ionic liquid-loaded Fe3O4@SiO2 magnetic catalytic microspheres coupled with persulfate for catalytic oxidative desulfurization

Functional ionic liquid loading magnetic Fe3O4@SiO2 microspheres with persulfate were applied to desulfurization.

Swelling Behavior and Flow Rates of a Novel Hydrophilic Gasket Used in Composite Geomembrane Vertical Cutoff Walls and Infrastructures Exposed to Contaminated Groundwater

The swelling capacity of novel hydrophilic gaskets used in geomembrane cutoff walls and infrastructures is critical for decreasing the flow rates of contaminated groundwater. This study investigated the swelling behavior, relaxation characteristics, flow rates, and micro-morphology of a hydrophilic gasket with different testing liquids. The radial swelling tests were performed using a device modified from single-lever consolidation instrument. A flow rates model apparatus was manufactured and employed to measure the flow rates of the poor-sealing hydrophilic gasket. According to the test results, the swelling ratio of the hydrophilic gaskets soaked in the DIW were the highest, followed by the NaCl solution, the MSW landfill leachate, and the CaCl2 solution. Relaxation phenomena appeared in all the specimens regardless of the testing liquids. The flow rates of the specimens penetrated with DIW, NaCl, and CaCl2 decreased to a stable state, and then increased extremely slowly to stable values. Moreover, self-healing of the hydrophilic gasket was observed. The micro-morphology indicated that sodium polyacrylate (PAAS) with insufficient expansion could separate from the matrix under high multivalent ionic strength or loading pressure conditions. Therefore, it is critical to develop the modified hydrophilic gasket with resistance to contaminated groundwater for a better barrier performance for use in contaminated sites and infrastructures.

Supported ionic liquid phase facilitated catalysis with lipase from Aspergillus oryzae for enhance enantiomeric resolution of racemic ibuprofen

Supported ionic liquid phase (SILP) was used as a carrier for lipase from Aspergillus oryzae (LAO) and used as a biocatalyst for enantiomeric resolution of racemic ibuprofen via esterification leading to (S) -(+)-ibuprofen ester. Using native form of lipase, outstanding results were achieved, obtaining (S) -(+)-ibuprofen propyl ester with enantiomeric excess ( ee ) of 99.9% and high conversion of racemic ibuprofen after 24 h ( α = 34 . 8 % ) and respectively ee = 99.9% with α = 45 . 2 % after 48 h. Several hybrid materials composited with silica and metal-based oxides including magnesium, calcium, and zirconia were evaluated as supports for LAO with various surface characteristics. The selected ionic liquid 1-methyl-3-(triethoxysilylpropyl)imidazolium bis(trifluoromethylsulfonyl)imide was immobilized via the covalent bound onto the surface of solid material and in the second step LAO was anchored. Optimized results in enantiomeric resolution of racemic ibuprofen (35.23% conversion of rac -ibuprofen after 7 days with 95% ee of ester) were obtained for SILP biocatalyst based on MgO ⋅ SiO 2 (1:1) (ionic liquid loading 6.79%, enzyme loading 3.96%). This is proposed as a generic approach to tailoring supported ionic liquids phase biocatalysts for industrially-relevant reactions, to generate both environmentally and economically sustainable processes. • Aspergillus oryzae lipase was used in enantiomeric resolution of racemic ibuprofen. • Free enzyme showed over 45% reaction yield and 99.9% enantiomeric excess after 48 h. • Supported ionic liquid phase with lipase was used to improve system feasibility. • Modification of surface with ionic liquid enabled efficient immobilization of enzyme. • High reaction rate and enantioselectivity were maintained in the reusability test.

Novel morphologies of mesoporous hierarchically assembled nanostructured hydroxyapatite particles: Influence of some synthesis conditions

Hierarchically assembled nanostructured apatitic (HANA) mesoporous particles have been hailed as potential drug delivery agents. However, their synthesis is intricate, and synthesis process parameters critically affect their formation. This investigation comprehensively evaluated the effects of both temperature and duration of hydrothermal heating on the architecture and structure of HANA particles. Variations in temperature and heating duration unfolded various HANA particle morphologies, including bundle-like, flower-like, dumbbell-like, and spherical-ended dumbbell-like particles. All morphologies exhibited monolithic apatitic structures with varying crystallinity and lattice strain. Also, particles exhibited mesoporous structures with superior surface area (16–23 m2g-1) and pore volume (0.009–0.048 cm3g-1). Spherical-ended dumbbell-like particles displayed strong drug encapsulation efficiency and improved pharmacokinetics in simulated body conditions based on their ionic release rate, drug loading, and release rate testings. Therefore, an amalgamation of amazing properties of HANA particles proposed their therapeutic applications as agents for controlled drug administration and tissue restoration multifunctions.

Bioinspired Semicrystalline Dynamic Ionogels with Adaptive Mechanics and Tactile Sensing.

A biological system shows dynamical shapes and tunable mechanical states while working as an actuator and/or sensor. To simulate this, we prepared semicrystalline dynamic ionogels (SDIGs) via a facile process by introducing crystallized polymer domains for phase change and amorphous domains for ionic liquid loading into ionogels. The obtained SDIGs offered tunable mechanical properties upon temperature switching with a change in modulus up to 2 orders of magnitude. It also showed an excellent shape memory effect, shape programmability, and melting accelerated conductivity increase. Enabled by ionic Joule heating technique, the ionogel provided an electrical triggered actuating process to mimic flower blossoming. Moreover, it was demonstrated as a touch sensor with various working shape states, indicating cyclic and green utilization. This work provides insights into the design of semicrystalline electronics and is believed to promote the development of biomimetic actuators and sensors.

Immobilization of acetate based ionic liquids on silica gel to fabricate a prospective desulfurizing adsorbent

ABSTRACT Ionic liquids have the potential to play a significant role in mitigating the critical challenge of refractory sulfur removal from diesel. In the present investigation, a mixture of imidazolium, pyrazolium and triazolium acetate -based ionic liquids has been immobilized on silica gel using sol-gel technology at ambient temperature (25°C), yielding a novel adsorbent. The sol-gel processing route has been elucidated by Dynamic Light Scattering (DLS) and rheology study. The fabricated adsorbent has been characterized by Fourier Transfer Infra-red (FTIR) spectroscopy, X-ray Diffraction (XRD) and Scanning Electron Microscopy (SEM). The results reveal that the ionic liquids have been immobilized in the silica gel support. This adsorbent has been successfully applied to remove heterocyclic sulfur compounds from model diesel containing thiophene and dibenzothiophene. The highest desulfurization efficiencies achieved for thiophene and dibenzothiophene removal are 98.31 and 99.29% respectively, using an adsorbent with 15% ionic liquid loading, model diesel: adsorbent ratio of 1:0.075, an adsorption time of 60 minutes at 25°C. The system under investigation followed the Langmuir isotherm model and the adsorption performance best fitted with the Ho’s pseudo second-order kinetics.

Unravelling the physiological basis of salinity stress tolerance in cultivated and wild rice species.

Wild rice species provide a rich source of genetic diversity for possible introgression of salinity stress tolerance in cultivated rice. We investigated the physiological basis of salinity stress tolerance in Oryza species by using six rice genotypes (Oryza sativa L.) and four wild rice species. Three weeks of salinity treatment significantly (P <0.05) reduced physiological and growth indices of all cultivated and wild rice lines. However, the impact of salinity-induced growth reduction differed substantially among accessions. Salt tolerant accessions showed better control over gas exchange properties, exhibited higher tissue tolerance, and retained higher potassium ion content despite higher sodium ion accumulation in leaves. Wild rice species showed relatively lower and steadier xylem sap sodium ion content over the period of 3weeks analysed, suggesting better control over ionic sodium xylem loading and its delivery to shoots with efficient vacuolar sodium ion sequestration. Contrary to this, saline sensitive genotypes managed to avoid initial Na+ loading but failed to accomplish this in the long term and showed higher sap sodium ion content. Conclusively, our results suggest that wild rice genotypes have more efficient control over xylem sodium ion loading, rely on tissue tolerance mechanisms and allow for a rapid osmotic adjustment by using sodium ions as cheap osmoticum for osmoregulation.

Impact of Ionic Liquid Structure and Loading on Gas Sorption and Permeation for ZIF-8-Based Composites and Mixed Matrix Membranes.

Carbon dioxide (CO2) capture has become of great importance for industrial processes due to the adverse environmental effects of gas emissions. Mixed matrix membranes (MMMs) have been studied as an alternative to traditional technologies, especially due to their potential to overcome the practical limitations of conventional polymeric and inorganic membranes. In this work, the effect of using different ionic liquids (ILs) with the stable metal–organic framework (MOF) ZIF-8 was evaluated. Several IL@ZIF-8 composites and IL@ZIF-8 MMMs were prepared to improve the selective CO2 sorption and permeation over other gases such as methane (CH4) and nitrogen (N2). Different ILs and two distinct loadings were prepared to study not only the effect of IL concentration, but also the impact of the IL structure and affinity towards a specific gas mixture separation. Single gas sorption studies showed an improvement in CO2/CH4 and CO2/N2 selectivities, compared with the ones for the pristine ZIF-8, increasing with IL loading. In addition, the prepared IL@ZIF-8 MMMs showed improved CO2 selective behavior and mechanical strength with respect to ZIF-8 MMMs, with a strong dependence on the intrinsic IL CO2 selectivity. Therefore, the selection of high affinity ILs can lead to the improvement of CO2 selective separation for IL@ZIF-8 MMMs.

Hybrid polymer/ionic liquid electrospun membranes with tunable surface charge for virus capture in aqueous environments

Although electrospun-based membranes may be engineered as efficient platforms for the capture of biomolecules in aqueous environments, the capability of such membranes to selectively capture viruses and proteins is often limited due to poor and constrained surface affinity for molecular bonding. In order to generate more efficient electrospun-based membranes, fine-tuning Van der Waals and ionic interactions is required to control chemical affinities with such contaminants and support advanced remediation solutions. Here, diallydimethylammonium chloride and poly(acrylonitrile) electrospun nanofibres were developed to enhance the adsorption of specific contaminant molecules compared to equivalently shaped pristine poly(acrylonitrile) nanofibre membranes. The results showed that the incorporation of the ionic liquid improved contact with water by forming super-hydrophilic nanofibres with narrow diameters and smaller pore size distributions, while also significantly changing the surface charge of the material and shifting the isoelectric point of the surface from 3 to 4.4. The specific surface area of the membranes was also increased by up to 4 times upon ionic liquid loading, which was found to support efficient coronavirus capture and filtration efficiency. This new strategy represents a promising way to control surface properties of virus filtration membranes towards efficient and targeted remediation solutions.

Natural Rubber/Carbon Nanotube/Ionic Liquid Composite Membranes: Vapor Permeation and Gas Permeability Properties

AbstractNatural rubber (NR)/carbon nanotube/ionic liquid nanocomposite membranes, prepared by using sulfur as the crosslinking agent, are tested for their vapor permeation (VP) characteristics. The permeation studies are conducted using three solvents, pentane, hexane and heptane as aliphatic solvents and toluene as aromatic solvent. The effects of the ionic liquid loading, CNT loading, and penetrant size on the vapor permeability of the membranes are investigated. The vapor permeability of the nanocomposite is found to increase with an increase in the ionic liquid content and decreases with CNT loading. Generally, cyclohexane is produced by the catalytical hydrogenation of benzene at high temperature. It is very difficult to purify it by removing unreacted benzene due to the close boiling point of cyclohexane and benzene and their azeotropic mixture formation tendency. By using NR/CNT/IL nanocomposite membrane, VP technique is applied for the separation of benzene/cyclohexane mixtures, including azeotropic composition of the solvents. The gas permeabilities of the NR, NR/CNT3, and NR/CNT3/IL membranes are determined with nitrogen and oxygen. Among these membranes, NR/CNT3/IL shows highest permeability. Compared to nitrogen, oxygen shows higher permeability.

The Impact of Ionic Liquid Loading in Three-Dimensional Carbon Nanotube Networks on the Separation of CO2/CH4 Fluid Mixtures: Insights from Molecular Simulations

The Impact of Ionic Liquid Loading in Three-Dimensional Carbon Nanotube Networks on the Separation of CO₂/CH₄ Fluid Mixtures: Insights from Molecular Simulations

Deciphering the Molecular Mechanism of Water Interaction with Gelatin Methacryloyl Hydrogels: Role of Ionic Strength, pH, Drug Loading and Hydrogel Network Characteristics.

Water plays a primary role in the functionality of biomedical polymers such as hydrogels. The state of water, defined as bound, intermediate, or free, and its molecular organization within hydrogels is an important factor governing biocompatibility and hemocompatibility. Here, we present a systematic study of water states in gelatin methacryloyl (GelMA) hydrogels designed for drug delivery and tissue engineering applications. We demonstrate that increasing ionic strength of the swelling media correlated with the proportion of non-freezable bound water. We attribute this to the capability of ions to create ion–dipole bonds with both the polymer and water, thereby reinforcing the first layer of polymer hydration. Both pH and ionic strength impacted the mesh size, having potential implications for drug delivery applications. The mechanical properties of GelMA hydrogels were largely unaffected by variations in ionic strength or pH. Loading of cefazolin, a small polar antibiotic molecule, led to a dose-dependent increase of non-freezable bound water, attributed to the drug’s capacity to form hydrogen bonds with water, which helped recruit water molecules in the hydrogels’ first hydration layer. This work enables a deeper understanding of water states and molecular arrangement at the hydrogel–polymer interface and how environmental cues influence them.