Hydrogen-bonded Water Research Articles

Di-μ3-chlorido-1:2:3κ3 Cl;2:3:4κ3 Cl-di-μ2-chlorido-1:2κ2 Cl;3:4κ2 Cl-tetrakis[(4-amino-1,5-dimethyl-2-phenyl-2,3-dihydro-1H-pyrazol-3-one-κ2 N 4,O)chloridocadmium(II)] 1.7-hydrate: a new six-coordinate geometry index, τ6

The title centrosymmetric tetranuclear cadmium(II) complex of 4-aminoantipyrine and chloride ions, [Cd4Cl8(C11H13N3O)4]·1.7H2O, was synthesized using methanol as solvent. The two independent Cd2+ ions in the asymmetric unit have different geometries; the outer Cd atoms have fivefold CdONCl3 coordination spheres, while the inner Cd atoms have sixfold CdONCl4 coordination spheres. The complex is consolidated by intramolecular N—H...O and N—H...Cl hydrogen bonds. In the crystal, a combination of N—H...Cl and Ow—H...Cl (w = water) hydrogen bonds link the components to form chains propagating along the a-axis direction. The chains are crosslinked by C—H...Cl and C—H...O hydrogen bonds to form a three-dimensional structure. A new geometry index, τ6, is proposed to quantitatively estimate the geometry of a sixfold coordinated atom.

Water Cooperativity Impacts Aromatic Interactions in the Aggregation of Benzene with Water.

The interactions between water and aromatic rings are pervasive across various scientific and technological disciplines, including biochemistry, materials science, and environmental chemistry. In this study, we combine broadband rotational spectroscopy and quantum-chemical calculations to reveal detailed structural and binding motifs in the aggregation of benzene, as the prototypical aromatic molecule, in the presence of a few water molecules. The benzene dimer and trimer structures with up to two water molecules are conclusively identified through isotopic substitution. We observe that the π-stacking interactions are substituted by more favorable CH···π contacts, allowing the insertion of water molecules acting as bridges between aromatic rings. This induces a shortening of the O···O distances for the complexes with two water molecules compared to that of the isolated water dimer. A many-body decomposition analysis of the interaction energy reveals the interactions of water with the aromatic partners through three-body contributions. While in the prototypical hydrogen-bonded pure water clusters this contribution amounts to 20-25% of the total interaction energy, we observe a significant contribution on the order of 10% in the interactions with the benzene rings. These results experimentally rationalize the binding strength of π-systems with water.

Experimental quantification of nuclear quantum effects on the hydrogen bond of liquid water

Nuclear quantum effects (NQEs) significantly influence material properties upon isotopic substitution, particularly with light atoms such as hydrogen. While water is rich in hydrogen, its hydrogen-bonded structure exhibits only moderate NQEs. Simulations ascribe this to competing zero-point energies (ZPEs): Intermolecular ZPEs stabilize hydrogen-bonds, while intramolecular ZPEs destabilize them. However, experimental validation has been lacking due to the difficulty in quantifying NQEs. The air/water interface provides an ideal platform to quantify NQEs in liquid water using surface-specific vibrational spectroscopy. By analyzing the excess/depletion of interfacial HOD, H 2 O, and D 2 O molecules with one free OH/OD group and the other H-bonded OH/OD group, we found that the intermolecular ZPE destabilizes the hydrogen-bonds by 0.74 ± 0.20 kilojoule per mole upon isotope substitution from H to D, while the intramolecular ZPE stabilizes them by 0.78 ± 0.33 kilojoule per mole. This near-complete cancellation explains the overall moderate NQE in liquid water. The interface thus allows for quantifying NQEs in water.

Selective Aliphatic Aldimine Formation and Stabilization by a Hydrophobic Capsule in Water.

Imines and enamines are useful intermediates in biochemical aldol-type reactions since their acid/base characteristics are accessible near neutrality. However, the generation of aldimines in water is a challenge as the equilibrium favors the components alkyl amines and aldehydes. Here, we report the generation, recognition, and protection of aldimines accomplished by a water-soluble capsule. The capsule provides a well-defined hydrophobic cavity isolating aldimines from the medium by a dry seam of Se-N chalcogen bonds instead of a wet seam of hydrogen bonds in water. A series of diverse aldimines are formed in situ and trapped rapidly (within 45 min at mM concentrations) in D2O with more than 90% yields. The encapsulated aldimines are stable for at least one month under ambient conditions. The aliphatic aldimines are selectively formed in the capsule even though they are less stable than aromatic imines in solution. The aldimines can be released from the capsule containers by competitive guests such as adamantane.

The interface hydrophilic-hydrophobic integration of fluorinated defective graphene towards biomedical applications.

In biomedical fields, rational design of novel two-dimensional (2D) biomedical nanomaterials aims to precisely manipulate biomolecules, including efficient capture, structural-functional transformation, directional movement, and self-assembly. In this work, we innovatively proposed new graphene nanosheets and selected two representative proteins to explore their binding mechanisms, structural-functional transformation of proteins, and biological effects of the materials. Fluorinated defective graphene (FDG) exhibited highly efficient capture and structural-functional transformation for the receptor binding domain (RBD), and we observed its collapse phenomenon in 2D materials for the first time. For the main protease (Mpro), FDG achieved an optimal balance between efficient capture, immobilization, and structural disruption. Further studies showed that fluorination on oxygen-containing defect graphene significantly enhanced variances in water distribution, surface properties, and hydrogen bond networks on the material surface. This allowed amino acids to be confined to specific areas, achieving efficient capture and directional movement. Additionally, the adsorption behavior and interaction strength of peptides and deoxynucleotides on FDG further validated the possibility of self-assembly. In summary, we highlight FDG as an excellent biomedical material with hydrophilic-hydrophobic integration.

Role of Interfacial Water in Improving the Activity and Stability of Lattice-Oxygen-Mediated Acidic Oxygen Evolution on RuO2.

Although RuO2-based electrocatalysts have been widely studied for acidic oxygen evolution reaction (OER), triggering the conventional adsorbate evolution mechanism to suppress kinetically favorable lattice oxygen mechanism (LOM) pathway at the expense of activity is the state-of-the-art strategy. To date, approaches to simultaneously achieve remarkable activity and stability of RuO2-based electrocatalysts through the kinetically favorable LOM pathway toward acidic OER are still elusive. Herein, we report that RuS0.45Ox catalyst with the synergetic regulation of asymmetric S-Ru-O microstructure and Ru-SO4 local environments can simultaneously boost the lattice-oxygen-mediated OER activity and stability under acidic electrolyte. Experimental results, including operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy, operando X-ray photoelectron spectroscopy, and theoretical studies, indicate the dynamic evolution of interfacial water structure from hydrogen-bond water to free-H2O on the surface of RuS0.45Ox. The generated continuous free-H2O-enriched local environment is in favor of accelerating the sluggish kinetics of interfacial water dissociation and facilitating the replenishment of lattice oxygen vacancies generated during the lattice-oxygen-mediated OER process, thereby significantly enhancing the stability. Consequently, the obtained RuS0.45Ox displays remarkable acidic OER performance with 160mV to reach 10mA cm-2, and robust stability with negligible activity decay over 500 h at 100mA cm-2.

Solubility and thermodynamic interactions of L-aspartic acid in aqueous organic solvent systems

This study examines the complex behavior of L-aspartic acid in water-organic solvent systems, namely its solubility and thermodynamic interactions across a range of temperatures. L-aspartic acid, a vital component in protein synthesis and cellular processes, exhibits various solubility patterns influenced by solvent properties and structural features. Experimental methods involving gravimetric analysis were employed to measure solubility, revealing temperature-dependent trends. Results indicate that L-aspartic acid solubility increases with rise in temperature, with the highest solubility observed in pure water and lower solubility observed in organic media. Notably, L-aspartic acid shows significant solubility in water–dimethylformamide (DMF) systems owing to favorable dipole–dipole interactions. However, solubility diminishes in water–acetonitrile (ACN) systems, attributed to ACN’s hydrophobic nature. Thermodynamic analysis reveals complex interactions, including hydrogen bonding and dipole-dipole forces, impacting solvation. Furthermore, the role of L-aspartic acid is evaluated in solvent–solvent interactions, elucidating the changes in entropy and solvent structure. The introduction of L-aspartic acid disrupts intermolecular hydrogen bonds in water, leading to increased disorder. Conversely, the water-organic solvent systems exhibit structured arrays, influenced by acid–base interactions and solvent self-association. Overall, this investigation provides insights into the thermodynamic behavior of L-aspartic acid in mixed solvent systems, shedding light on its applications in biological and industrial realms. Further researches will elucidate the complex interactions.

Optical Absorption Spectroscopy Probes Water Wire and Its Ordering in a Hydrogen-Bond Network

Water wires, quasi-one-dimensional chains composed of hydrogen-bonded (H-bonded) water molecules, play a fundamental role in numerous chemical, physical, and physiological processes. Yet direct experimental detection of water wires has been elusive so far. Based on advanced many-body theory that includes electron-hole interactions, we report that optical absorption spectroscopy can serve as a sensitive probe of water wires and their ordering. In both liquid and solid water, the main peak of the spectrum is discovered to be a charge-transfer exciton. In water, the charge-transfer exciton is strongly coupled to the H-bonding environment where the exciton is excited between H-bonded water molecules with a large spectral intensity. In regular ice, the spectral weight of the charge-transfer exciton is enhanced by a collective excitation occurring on proton-ordered water wires, whose spectral intensity scales with the ordering length of water wire. The spectral intensity and excitonic interaction strength reaches its maximum in ice XI, where the long-range ordering length yields the most pronounced spectral signal. Our findings suggest that water wires, which widely exist in important physiological and biological systems and other phases of ice, can be directly probed by this approach. Published by the American Physical Society 2025

Protein modifications and ionic strength show the difference between protein-mediated and solvent-mediated regulation of biomolecular condensation

Biomolecular condensation is an important mechanism of cellular compartmentalization without membranes. Formation of liquid-like condensates of biomolecules involves protein-protein interactions working in tandem with protein-water interactions. The balance of these interactions in condensate-forming proteins is impacted by multiple factors inside of a living organism. This work investigates the effects of post-translational modifications (PTMs) and salt concentration as two such perturbing factors on the protein Fused in Sarcoma (FUS), an RNA binding protein. The protein was obtained from two expression systems differing by their capability to add PTMs to the protein, bacterial and insect cell. Attenuated total reflection Terahertz spectroscopy is used to probe the solvation behavior in condensates formed from FUS protein with and without PTMs at 100 mM and 2.5 M KCl. The results show that while PTMs impact the phase-separating propensity, they do not alter protein solvation in the condensate. On the other hand, salt concentration was found to alter the stiffness of the water hydrogen bond network. These findings have implications for biomolecular condensates chemistry, showing that condensate molecular organization is perturbed by fluctuations in solvent properties.

Efficient Electrocatalytic Semi-Hydrogenation of Alkynes by Interfacial Engineering of Atomically Precise Silver Nanoclusters.

Owing to its green energy and hydrogen sources, electrocatalytic semi-hydrogenation of alkynes is an attractive alternative for industrial alkene production. However, its broad application is hindered by low selectivity and low Faradaic efficiency (FE) due to side reactions like over-hydrogenation to alkanes. Here, we demonstrate that atomically precise Ag25(MHA)18 nanoclusters (NCs) can electrocatalyze alkyne semi-hydrogenation with 98% conversion, 99% selectivity, and 85% FE, in a broad substrate pool. This is achieved by engineering the local environment at the catalytically active sites. We leverage amphiphilic MHA (6-mercaptohexanoic acid) ligands to pre-concentrate water molecules and alkynes near the ligand-layer/Ag25 interface. Long-chain ligands can disrupt the hydrogen-bond network at the interface, the high negative charge of Ag25 can attract weakly hydrogen-bonded water through counterions and promote the generation of active hydrogen (H*), while the enzyme-like catalytic pockets on the surface of Ag25 NCs facilitate adsorption of terminal alkynes via σ-bonding to the surface Ag atoms. Density functional theory calculations confirmed the preference of the σ-bonding model of alkyne and further revealed the facile release of product alkene. This work exemplifies an atomically precise interface engineering strategy to control the local environment of active sites for optimized activity and selectivity.

Confined Structural Water Molecules as Alternative Potential Emitters for Bright Photoluminescence of Thiolate-Gold Complexes.

The debate about water as an emitter has spanned nearly a century, but how it emits bright colors remains elusive. In this report, using the widely used Au(I)-alkanethiolate complex (Au(I)-SRs, R=-(CH2)12H) with AIE properties as a model system, by carefully manipulating the delicate surface-ligand interactions at the nanoscale interface, together with a careful spectral investigation and an isotopic diagnostic experiment of heavy water (D2O), we demonstrated that the structural water molecules (SWs) trapped in the nanoscale interface or space are the true emission centers of metal nanoclusters (NCs) and the aggregates of Au(I)-SRs complexes, instead of a well-organized metal core dominated by quantum confinement mechanics. Unlike conventional hydrogen-bonded water molecules, due to interfacial adsorption or spatial confinement, the p-orbitals of two O atoms in SWs can form strong electronic interactions through spatial overlap, thus constructing a set of interfacial states, one of which is characterized by π-bonding, thus providing alternative channels (or paths) for the relaxation decay of the excited electrons. Using the one-dimensional free-electron gas model, the energy levels calculated by the Schrödinger equation are in perfect agreement with the experimental observations, further validating the SWs model.

Alkali Halide Aqueous Solutions Under Pressure: A Non-Equilibrium Molecular Dynamics Investigation of Thermal Transport and Thermodiffusion.

Thermal gradients induce thermodiffusion in aqueous solutions, a non-equilibrium effect arising from the coupling of thermal and mass fluxes. While thermal transport processes have garnered significant attention under standard conditions, thermal transport at high pressures and temperatures, typical of the Earth's crust, has escaped scrutiny. Non-equilibrium thermodynamics theory and non-equilibrium molecular dynamics simulations provide an excellent means to quantify thermal transport under extreme conditions and establish a connection between the behaviour of the solutions and their microscopic structure. Here, we investigate the thermal conductivity and thermal diffusion of NaCl and LiCl solutions in the GPa pressure regime, targeting temperatures between 300 K and 1000 K at 1 molal concentration. We employ non-equilibrium molecular dynamics simulations along with the Madrid-2019 and TIP4P/2005 force fields. The thermal conductivity of the solutions increases significantly with pressure, and following the behaviour observed at standard pressure, the thermal conductivity is lower than that of pure water. The reduction in thermal conductivity is significant in the GPa pressure regime, ∼3% for 1 molal NaCl and LiCl solutions. We demonstrate that under GPa pressure conditions, the solutions feature thermophobic behaviour, with ions migrating towards colder regions. The pronounced impact of pressure is more evident in LiCl solutions, which display a thermophilic to thermophobic "transition" at pressures above 0.25 GPa. We discuss a correlation between the solution's thermophobicity and the disruption of the water hydrogen bond structure at high pressure, where the water structure resembles that observed in simple liquids.

Insights on Hydrogen Bond Network of Water in Phospholipid Membranes: An Infrared Study at Varying Hydration.

Water in membrane interphases is vital for cellular biological functions, but despite its importance, the structure and function of biological water remain elusive. Here, by studying the OH stretching mode in partially hydrated lipid multilayers by FTIR measurements, relevant information on the water structure near the surface with lipid membranes has been gathered. The water hydrogen bond network is highly perturbed in the first layers that are in contact with the lipid membrane, exhibiting strong deviations from tetrahedral symmetry and a significant number of defects, such as isolated water molecules and a large number of hydrogen-bonded water dimers in the interphase region. These findings support the hypothesis that water chains form in phospholipid membranes, and are involved in the proton transfer across lipid bilayers by phosphate groups of opposing lipids. Furthermore, we have determined that even at very low hydration levels, a small amount of water is embedded within the confined spaces of the hydrocarbon region of phospholipid bilayers, which could potentially contribute to the structural stability of the lipid membrane.

Understanding the protein conformation transition within polymer hydrogels using a near-infrared water spectroscopy probe.

Understanding the protein conformation transition within polymer hydrogels using a near-infrared water spectroscopy probe.

Photochemistry of Microsolvated Nitrous Acid: Observation of the Water-Separated Complex of Nitric Oxide and Hydroxyl Radical.

The photochemistry of nitrous acid (HONO) plays a crucial role in atmospheric chemistry as it serves as a key source of hydroxyl radicals (OH) in the atmosphere; however, our comprehension of the underlying mechanism for the photochemistry of HONO especially in the presence of water is far from being complete as the transient intermediates in the photoreactions have not been observed. Herein, we report the photochemistry of microsolvated HONO by water in a cryogenic N2 matrix. Specifically, the 1:1 hydrogen-bonded water complex of HONO was facially prepared in the matrix through stepwise photolytic O2 oxidation of the water complex of imidogen (NH-H2O) via the intermediacy of the elusive water complex of peroxyl isomer HNOO. Upon photolysis at 193 nm, the matrix-isolated HONO-H2O complex decomposes by yielding the ternary water complex of OH and NO due to the matrix cage effect. The identification of this rare water-separated radical pair (OH-H2O-NO) with matrix-isolation infrared and ultraviolet-visible spectroscopy is aided by D, 15N, and 18O isotope labeling and quantum chemical calculations at the (U)CCSD/AVTZ level of theory, and its most stable structure exhibits separate hydrogen bonding interactions of the OH and NO radicals with H2O via OH···OH2 and ON···HOH contacts, respectively. This ternary complex is extremely unstable, as it undergoes spontaneous radical recombination to reform the HONO-H2O complex in the temperature range of 4-12 K through quantum-mechanical tunneling with 16/18O, H/D, 14/15N kinetic isotopic effects of 1.43, 2.33, and 0.91, respectively. At increased temperatures from 15 to 21 K, the recombination proceeds predominantly by overcoming the activation barrier with an estimated height of 0.12(1) kcal/mol.

Molecular Dynamics Simulation of Clay Mineral–Water Interfaces: Temperature-Dependent Structural, Dynamical, and Mechanical Properties

Water interacting with clay minerals—such as kaolinite, montmorillonite, and pyrophyllite—fundamentally governs their geotechnical and environmental functions, thereby influencing parameters such as retention, transport, and stability. Understanding the effects of temperature on water behavior within clay mineral interlayers is critical for predicting the performance of clay–water systems under dynamic environmental conditions. This study performed molecular dynamics simulations to investigate the structural, dynamical, and mechanical properties of interlayer water in three representative clay minerals over a temperature range of 298.15–363.15 K. Our analyses focused on mean squared displacement (MSD), density profiles, hydrogen bond dynamics, and stress distributions, thereby revealing the interaction between water structuring and thermal fluctuations. Results indicated distinct temperature-dependent changes in water diffusion and hydrogen bond stability, with montmorillonite consistently exhibiting enhanced water retention and steadier hydrogen bonding networks across the studied temperature spectrum. Density profiles highlighted pronounced confinement effects at lower temperatures that gradually diminish with increasing thermal energy. Concurrently, the stress distributions revealed the mechanical responses of clay–water interfaces, highlighting the interplay between thermal motion of water molecules and their interactions with the clay surfaces. These findings offer valuable insights into how temperature regulates water behavior in clay mineral interlayers and provide a foundation for advancing predictive modeling and the design of engineered systems in water-rich, thermally variable environments.

Influence of CTAB Reverse Micellar Confinement on the Tetrahedral Structure of Liquid Water.

The effect of confinement on the tetrahedral ordering of liquid water plays a vital role in controlling their microscopic structure and dynamics as well as their spectroscopic properties. In this article, we have performed the classical molecular dynamics simulations of four different CTAB/water/chloroform reverse micelles with varied water content to study how the tetrahedral ordering of nanoscale water inside reverse micellar confinement influences the microscopic dynamics and the structural relaxation of water···water hydrogen bonds and its impact on the low-frequency intermolecular vibrational bands. We have noticed from the results obtained from simulated trajectories the lowering trends of tetrahedral ordering of water pools in reverse micellar confinements as we move from bulk to confined and strictly confined environments. We have observed that the order of confinements significantly altered the relaxation pattern of water···water hydrogen bonds present in the nanoscale water pool of reverse micelles. The recrossing related to hydrogen bond dynamics can effectively explain the relaxation pattern of under confinement. The Br-1···water hydrogen bond depicts a much slower relaxation compared to the water···water hydrogen bonds inside reverse micelles. We have also explored the correlation between the tetrahedral ordering of nanoscale water pools and the relaxation of water···water hydrogen bonds with the 50 cm-1 band for water inside reverse micelles. The computations reported that compared to bulk water, the band appearing at 50 cm-1 for O···O···O triplet bending is nonuniformly blue-shifted by 18-45 cm-1 for the nanoscale water pool inside reverse micelles, and the intensity of the band drops from bulk to confined and strictly confined environments, which indicates the reduced tendency of such triplet formation. It is observed that a significant intensity variation at the 200 cm-1 band correlates with the effect of confinement on the tetrahedral ordering of the water pool inside reverse micelles. So, our observations support the influence of strictly confined environments on the tetrahedral water structure to adopt the quasi-two-dimensional water network and experience restricted longitudinal translations. It is further noticed that the 500 cm-1 librational band is also found to be blue-shifted by 71-112 cm-1 for the water pool in reverse micelles, and the extent of the shift being more noticeable for strictly confined environments correlates excellently with the sluggish relaxation of water···water hydrogen bonds in such environments.

Quasiphase transition of a single-file water chain influenced by atomic charges in a water model using orientational-biased replica exchange Monte Carlo simulations.

The recently observed temperature-dependent quasiphase transition of the single-file water chain confined within a carbon nanotube in experiments has been validated by the simple lattice theory and molecular dynamics simulations. It has been pointed out that the atomic charges in water models are important, yet how the values will affect the structural details and thermodynamic properties of the quasiphase transition has not been fully revealed. In this work we perform orientational-biased replica exchange Monte Carlo simulations in the canonical ensemble to explore the effect of atomic charges in the SPC/E water model on the quasiphase transition of a single-file water chain. Based on the atomic charge values reported in literature, three distinct quasiphases are reproduced, comprising a fully hydrogen-bonded water chain at lower temperatures, a more ordered dipolar orientation along the tube axis at intermediate temperatures, and a completely disordered structure at higher temperatures. Then by increasing the atomic charge values, we find that the fragmentation of the entire water chain into shorter water segments, the orientational ordering of water dipoles along the tube axis, and the transition towards complete disorder are all inhibited. Consequently, the transition temperatures between three quasiphases have been shifted to higher temperatures. The thermodynamic analysis demonstrates that the increased atomic charge values enhance the hydrogen bonding between neighboring water molecules and also the electrostatic attraction within the water chain, leading to a longer water dipole correlation length even at higher temperatures. These findings highlight the vital role of atomic charges in water models and also the electrostatic interaction in regulating the orientational ordering of water molecules under nanoconfinement.

Hydrogen-bond disruption in molecularly engineered Janus evaporators for enhanced solar desalination.

Hydrogels have emerged as effective evaporator platforms, significantly enhancing evaporation rates by disrupting water's hydrogen bond network. Here, we present an advanced strategy to improve hydrogel evaporation performance by tailoring alkyl hydrophobic groups within biparental polyelectrolyte-shell micelles grafted onto the polyvinyl alcohol (PVA) hydrogel surface. Poly(2-(diethylamino)ethyl methacrylate) (PDEAEMA) quaternized with methyl iodide (MeI) or ethyl iodide (EtI) formed the biparental polyelectrolyte shell, while poly(benzyl methacrylate) (PBzMA) constituted the micelle core, creating BE-MeI and BE-EtI micelles, respectively. The molecularly engineered BE-MeI micelles exhibited an optimized configuration of quaternary amines linked to hydrophobic groups, achieving a synergistic balance between water attraction via electrostatic interactions and water repulsion via steric hindrance. This configuration effectively disrupted the water's hydrogen bond network, lowering the water evaporation enthalpy to 1434 J g-1. The BE-MeI micelle-grafted PVA hydrogel achieved a record-breaking evaporation rate of 4.1 kg m-2 h-1 under 1 sun irradiation, surpassing prior benchmarks, including our previously reported poly(4-vinyl pyridine) quaternized by a MeI system. Additionally, the grafted micelle layer exhibited a salt rejection ratio of 99.62%, ensuring excellent desalination performance. The biparental polyelectrolyte-shell micelle grafting strategy is broadly applicable across diverse hydrogel systems, representing a significant advancement in solar-driven desalination technology.

Environmentally tolerant multifunctional eutectogel for highly sensitive wearable sensors.

Flexible hydrogel sensors have found extensive applications. However, the insufficient sensing sensitivity and the propensity to freeze at low temperatures restrict their use, particularly in frigid conditions. Herein, a multifunctional eutectogel with high transparency, anti-freezing, anti-swelling, adhesive, and self-healing properties is prepared by a one-step photopolymerization of acrylic acid and lauryl methacrylate in a binary solvent comprising water and deep eutectic solvent (DES). The results from the molecular dynamics simulations and density functional theory indicate that the hydrogen bonds between DES and water mixtures possess better stability than those between water molecules. On the other hand, DES breaks down hydrogen bonds in water, providing eutectogels with excellent anti-freezing even at -60 °C. Cetyltrimethylammonium bromide is incorporated to establish stable hydrophobic interactions and electrostatic attractions with polymer chains in the eutectogel network, resulting in superior mechanical (elongation at break of 2890%) and anti-swelling (only 2% swelling in water over 7 days) properties. The eutectogel-based strain sensors exhibit remarkable sensitivity, achieving a gauge factor of up to 15.4. The multifunctional eutectogel sensors can monitor motion and transmit encrypted information at low temperatures, demonstrating considerable potential for applications in flexible electronics within low-temperature environments.