Hydrogen Bond Network Of Water Research Articles

Strong Replaces Weak: ​Hydrogen Bond-Anchored Electrolyte Enabling Ultra-Stable and Wide-Temperature Aqueous Zinc-Ion Capacitors.

Despite aqueous electrolytes offer a great opportunity for large-scale energy storage owing to their safety and cost-effectiveness, their practical application suffers from the parasitic side reactions and poor temperature adaptability stemming from weak hydrogen-bond (HB) network in free water. Here, we propose the guiding thought "strong replaces weak" to design hydrogen bond-anchored electrolyte by introducing sulfolane (SL) for disrupting the regular weak HB network and contributing to superior temperature tolerance. Judiciously combined experimental characterization and theoretical calculation confirm that SL can remodel the primary solvation shell of metal ions, customize stable electrode interface chemistry and restrain the side reactions. Consequently, symmetric supercapacitor constructed by activated carbon (AC) electrodes is able to fully work within a voltage range of 2.4 V and reach high capacitance retention of 89.8% after 60000 cycles. Additionally, Zn anodes exhibit ultra-stable Zn plating/stripping behaviors and a wide temperature range (-20 ~ 60 °C), and zinc-ion capacitor (Zn//AC) also delivers an excellent cycling stability with capacity retention of 99.7% after 55000 cycles, implying that the designed electrolyte has practical application potential in extreme environments. This work proposes a novel critical solvation strategy that paves the route for the construction of ultra-stable and wide-temperature aqueous energy storage devices.

The effect of dilution on the energy dissipation in water interstellar ice analogues

Context. Interstellar ices and their energetic processing play an important role in advancing the chemical complexity in space. Interstellar ices covering dust grains are intrinsically mixed, and it is assumed that physicochemical changes induced by energetic processing – triggered by photons, electrons, and ions – strongly depend on the content of the ice. Yet, the modelling of these complex mixed systems in experiments and theory is complicated. Aims. In this paper, we investigate the effect of infrared irradiation on a series of different molecules mixed with porous amorphous solid water (pASW) to study the release of vibrational energy in the hydrogen-bonding network of water as a function of mixing ratio and ice content. Particularly, we select mixtures of 20:1 H2O:X and 5:1 H2O:X with X=CO2, NH3, or CH4. Methods. Infrared radiation was supplied by the intense and tunable free electron laser (FEL) 2 at the HFML-FELIX facility. We monitored the structural changes in the interstellar ice analogue after resonant infrared excitation using Fourier-transform reflection absorption infrared (FT-RAIR) spectroscopy. Results. We observed that on-resonance irradiation at the OH-stretching vibration of pASW results in quantitatively identical changes compared to pure pASW for all investigated mixtures. The structural changes we observed closely resemble the previously reported local reordering. The 5:1 mixtures show weaker changes compared to pure pASW, with a decrease in strength from NH3 to CO2. Conclusions. Since the hydrogen-bonding network of pASW restructures similarly upon FEL irradiation, regardless of the mixing component, treating ice layers in models that simulate energy dissipation in the hydrogen-bonding network as pure H2O ice layers can be a justified approximation. Hence, complex systems might not always be necessary to describe the infrared energetic processing of ices.

Probing atomic-scale processes at the ferrihydrite-water interface with reactive molecular dynamics

Interfacial processes involving metal (oxyhydr)oxide phases are important for the mobility and bioavailability of nutrients and contaminants in soils, sediments, and water. Consequently, these processes influence ecosystem health and functioning, and have shaped the biological and environmental co-evolution of Earth over geologic time. Here we employ reactive molecular dynamics simulations, supported by synchrotron X-ray spectroscopy to study the molecular-scale interfacial processes that influence surface complexation in ferrihydrite-water systems containing aqueous MoO42-\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\ ext {MoO}_4}^{2-}$$\\end{document}. We validate the utility of this approach by calculating surface complexation models directly from simulations. The reactive force-field captures the realistic dynamics of surface restructuring, surface charge equilibration, and the evolution of the interfacial water hydrogen bond network in response to adsorption and proton transfer. We find that upon hydration and adsorption, ferrihydrite restructures into a more disordered phase through surface charge equilibration, as revealed by simulations and high-resolution X-ray diffraction. We observed how this restructuring leads to a different interfacial hydrogen bond network compared to bulk water by monitoring water dynamics. Using umbrella sampling, we constructed the free energy landscape of aqueous MoO42-\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\ ext {MoO}_4}^{2-}$$\\end{document} adsorption at various concentrations and the deprotonation of the ferrihydrite surface. The results demonstrate excellent agreement with the values reported by experimental surface complexation models. These findings are important as reactive molecular dynamics opens new avenues to study mineral-water interfaces, enriching and refining surface complexation models beyond their foundational assumptions.Graphic

Hydroxyl-Binding Induced Hydrogen Bond Network Connectivity on Ru-based Catalysts for Efficient Alkaline Hydrogen Oxidation Electrocatalysis.

Understanding the role of adsorbed intermediates at the polarized catalyst-electrolyte interface on the structure of electrical double layer (EDL) is essential for developing highly efficient electrocatalysts. Here, we prepared a series of unconventional face-centered-cubic (fcc) phase Ru-based catalysts (i.e. fcc-Ru, fcc-RuCr, and fcc-RuCrW) by rational tuning the binding energetics of hydroxyl intermediate to engineer the electrochemical interface and boost the performance of alkaline hydrogen oxidation reaction (HOR). The introduction of oxyphilic metals Cr and W can regulate the orbital occupation of Ru, promote the adsorption of hydroxyl species, resulting in an anomalous behavior that HOR performance under alkaline media exceeds acidic media. Experimental results and theoretical calculations unravel that the modulated adsorption of hydroxyl species on the electrode surface are responsible for the reconstruction of interfacial water structure and dynamic evolution of free water molecules from nearest to the electrode surface to above the gap region in the EDL, thereby leading to significantly increased water connectivity and hydrogen bond network. Our work reveals a new understanding of the surface intermediates in controlling the dynamic process of interfacial water and hydrogen bonding network in HOR electrocatalysis, and will guide rational design of advanced electrocatalysts through electrochemical interfacial engineering.

Hydroxyl‐Binding Induced Hydrogen Bond Network Connectivity on Ru‐based Catalysts for Efficient Alkaline Hydrogen Oxidation Electrocatalysis

Understanding the role of adsorbed intermediates at the polarized catalyst‐electrolyte interface on the structure of electrical double layer (EDL) is essential for developing highly efficient electrocatalysts. Here, we prepared a series of unconventional face‐centered‐cubic (fcc) phase Ru‐based catalysts (i.e. fcc‐Ru, fcc‐RuCr, and fcc‐RuCrW) by rational tuning the binding energetics of hydroxyl intermediate to engineer the electrochemical interface and boost the performance of alkaline hydrogen oxidation reaction (HOR). The introduction of oxyphilic metals Cr and W can regulate the orbital occupation of Ru, promote the adsorption of hydroxyl species, resulting in an anomalous behavior that HOR performance under alkaline media exceeds acidic media. Experimental results and theoretical calculations unravel that the modulated adsorption of hydroxyl species on the electrode surface are responsible for the reconstruction of interfacial water structure and dynamic evolution of free water molecules from nearest to the electrode surface to above the gap region in the EDL, thereby leading to significantly increased water connectivity and hydrogen bond network. Our work reveals a new understanding of the surface intermediates in controlling the dynamic process of interfacial water and hydrogen bonding network in HOR electrocatalysis, and will guide rational design of advanced electrocatalysts through electrochemical interfacial engineering.

Dissecting the hydrogen bond network of water: Charge transfer and nuclear quantum effects

The molecular structure of water is dynamic, with intermolecular (H)-bond interactions being modified by both electronic charge transfer and nuclear quantum effects (NQEs). Electronic charge transfer and NQEs potentially change under acidic / basic conditions, but such details have not been measured. Here, we developed correlated vibrational spectroscopy, a symmetry-based method that distinctively separates interacting from non-interacting molecules in self- and cross-correlation spectra, giving access to previously inaccessible information. We found that OH − donated ~8% more negative charge to the H-bond network of water and H 3 O + accepted ~4% less negative charge from the H-bond network of water. D 2 O had ~9% more H-bonds compared to H 2 O, and acidic solutions displayed more dominant NQEs than basic ones.

Hydrogel Electrolyte with Regulated Water Activity and Hydrogen Bond Network for Ultra‐Stable Zinc Electrode

AbstractQuasi‐solid‐state zinc‐ion batteries (QZIBs) have attracted wide attention due to their excellent dimensional stability and high safety. However, poor ion conduction capabilities, severe dendrite growth, and rampant side reactions still hinder their commercialization. The regulation of the solvation structure of Zn2+ is considered to be an effective method to address these issues. Herein, a hydrogel electrolyte with a regulated solvation structure (HE‐RS) is designed via the combination of tetramethyl urea (TMU) additive and polyvinyl alcohol (PVA) matrix. The hydrophilic ─C═O group of TMU exhibits strong affinity with the PVA chains, improving the mechanical strength of the PVA matrix. The ─N(CH3)2 groups at both ends of TMU exhibit strong hydrophobic characteristics, which leads to local hydrophobicity and decreased water activity. Additionally, abundant oxygen‐containing (electronegative) groups on both PVA and TUM can adsorb Zn2+ and provide sites for Zn2+ transference. Benefiting from these merits, Zn2+ solvation structure and deposition behavior are regulated. Consequently, the Zn||Zn symmetric cell with HE‐RS exhibits a stable cycling life exceeding 2000 h. Moreover, the HE‐RS‐based Zn||NH4V4O10 cell exhibits a capacity retention of 96.4% after 1000 cycles at 2 A g−1.

Rational design of epoxy functionalized ionic liquids electrolyte additive for hydrogen-free and dendrite-free aqueous zinc batteries

Despite the high safety and low cost associated with aqueous Zn-ion batteries (ZIBs), uncontrolled Zn dendrite growth and parasitic reactions induced by water significantly diminish their stability. Herein, a new epoxy functionalized ionic liquid, 4-methyl-4-glycidylmorpholin bis[(trifluoromethyl)sulfonyl]imide (MGM[TFSI]), has been developed to mitigate water reactivity for stable ZIBs. It was found that the MGM+ cation disrupts the hydrogen bond network of water, hindering its adsorption on Zn anodes, thereby suppressing water decomposition and enhancing anode stability. Additionally, preferential adsorption of MGM+ cations on the Zn anode surface mitigates tip effects, suppresses dendrite growth, and promotes the formation of a ZnF2 solid electrolyte interphase layer, effectively isolating the anode from the bulk electrolyte. As a result, benefiting from the well-designed MGM+-based electrolyte, Zn//Zn cells achieve significantly enhanced cycling stability, lasting over 2000 h at 1 mA cm−2 with 1 mAh cm−2. Furthermore, Zn//MnO2 full cells deliver remarkable stability, retaining approximately 89 % of their initial capacity after 3000 cycles at 5 A/g. This work proposes that the MGM[TFSI] additive can effectively regulate the interfacial chemistry of the Zn anode, providing an opportunity to design advanced electrolytes for highly reversible ZIBs and beyond.

A structural determinant of the behavior of water at hydration and nanoconfinement conditions.

The molecular nature of the phases that conform the two-liquid scenario is elucidated in this work in the light of a molecular principle governing water structuring, which unveils the relevance of the contraction and reorientation of the second molecular shell to allow for the existence of coordination defects in water's hydrogen bond network. In turn, such principle is shown to also determine the behavior of hydration and nanoconfined water while enabling to define conditions for wettability (quantifying hydrophobicity and predicting drying transitions), thus opening the possibility to unravel the active role of water in central fields of research.

Can the AMOEBA forcefield be used for high pressure simulations? The extreme case of methane and water.

We have performed classical molecular dynamics simulations using the fully polarizable Atomic Multipole Optimized Energetics for Biomolecular Applications (AMOEBA) forcefield implemented within the Tinker package to determine whether a more adequate treatment of electrostatics is sufficient to correctly describe the mixing of methane with water under high pressure conditions. We found a significant difference between the ability of AMOEBA and other classical, computationally cheaper forcefields, such as TIP3P, simple point charge-extended, TIP4P, and optimized potentials for liquid simulations-all atom. While the latter models fail to detect any effect of pressure on the miscibility of methane in water, AMOEBA qualitatively captures the experimental observation of the increased solubility of methane in water with pressure. At higher temperatures, the solubility of water in methane also increases; this seems to be associated with the breakdown of the fourfold hydrogen-bonded water network structure: bonding in water is weaker, so the energy cost of solution is lowered.

Why Is Surface-Enhanced Raman Scattering Insensitive to Liquid Water?

Surface-enhanced Raman scattering (SERS) is widely recognized as a remarkably powerful analytical technique that enables trace-level detection of organic molecules on a metal surface in aqueous systems with negligible spectral interference of water. This insensitivity of SERS to liquid water is violated in a restrictive manner under specific electrochemical conditions. However, the origin of such different SERS sensitivities to liquid water remains unclear. Here, we show that hydrogen-bond networks of water play a pivotal role in losing SERS enhancement for liquid water, and SERS detection of water requires local defects in the hydrogen-bond networks, which are formed around hydration shells of solute ions or on a polarized electrode surface. This work gives a new perspective on in situ SERS investigations in aqueous systems, including electrochemical and biological reactions.

Hydrogen-Bonded Network of Water in Phase-Separated Biomolecular Condensates.

Biomolecular condensates formed via phase separation of intrinsically disordered proteins/regions (IDPs/IDRs) and nucleic acids are associated with cell physiology and disease. Water makes up for ∼60-70% of the condensate volume and is thought to influence the complex interplay of chain-chain and chain-solvent interactions, modulating the mesoscale properties of condensates. The behavior of water in condensates and the key roles of protein hydration water in driving the phase separation remain elusive. Here, we employ single-droplet vibrational Raman spectroscopy to illuminate the structural redistribution within protein hydration water during the phase separation of neuronal IDPs. Our Raman measurements reveal the changes in the water hydrogen bonding network during homotypic and heterotypic phase separation governed by various molecular drivers. Such single-droplet water Raman measurements offer a potent generic tool to unmask the intriguing interplay of sequence-encoded chain-chain and chain-solvent interactions governing macromolecular phase separation into membraneless organelles, synthetic condensates, and protocells.

Fluoro-Crown Ether Phosphate as Efficient Cell-Permeable Drug Carrier by Disrupting Hydration Layer.

Fast and direct permeation of drug molecules is crucial for effective biotherapeutics. Inspired by a recent finding that fluorous compounds disrupt the hydrogen-bonded network of water, we developed fluoro-crown ether phosphate CyclicFP-X. This compound acts as a fast cell-permeating agent, enabling direct delivery of various bioactive cargos (X) into cancer cells without endocytic entrapment. In contrast, its nonfluorinated cyclic analog (CyclicP-X) failed to achieve cellular internalization. Although the acyclic fluorous analog AcyclicFP-X was internalized, this process occurred slowly owing to the involvement of an endocytic trapping pathway. Designed with a high fluorine density, CyclicFP-X exhibits compactness, polarity, and high-water solubility, facilitating lipid vesicle fusion by disrupting their hydration layers. Raman spectroscopy confirmed the generation of dangling -OH bonds upon addition of CyclicFP-OH to water. Furthermore, conjugating CyclicFP-X with fluorouracil (FU, an anticancer drug) via a reductively cleavable disulfide linker (CyclicFP-SS-FU) demonstrated the general utility of fluoro-crown ether phosphate as a potent carrier for biotherapeutics.

Water Structure in the First Layers on TiO2: A Key Factor for Boosting Solar-Driven Water-Splitting Performances.

The water hydrogen-bonded network is strongly perturbed in the first layers in contact with the semiconductor surface. Even though this aspect influences the outer-sphere electron transfer, it was not recognized that it is a crucial factor impacting the solar-driven water-splitting performances. To fill this gap, we have selected two TiO2 anatase samples (with and without B-doping), and by extensive experimental and computational investigations, we have demonstrated that the remarkable 5-fold increase in water-splitting photoactivity of the B-doped sample cannot be ascribed to effects typically associated to enhanced photocatalytic properties, such as band gap, heterojunctions, crystal facets, and other aspects. Studying these samples by combining FTIR measurements under controlled humidity with first-principles simulations sheds light on the role and nature of the first-layer water structure in contact with the photocatalyst surfaces. It turns out that the doping hampers the percolation of tetrahedrally coordinated water molecules while enhancing the population of topological H-bond defects forming approximately linear H-bonded chains. This work unveils how doping the semiconductor surface affects the local electric field, determining the water splitting rate by influencing the H-bond topologies in the first water layers. This evidence opens new prospects for designing efficient photocatalysts for water splitting.

Catalytic Peculiarity of Alkali Metal Cation-Free Electrode/Polyelectrolyte Interfaces Toward CO2 Reduction.

A prominent feature of modern electrochemical technologies, such as fuel cells and electrolysis, is the employing of polyelectrolytes instead of liquid electrolytes. Unlike the well-studied electrode/liquid electrolyte interfaces, however, the catalytic characteristics of electrode/polyelectrolyte interfaces remain largely unexplored, mostly due to the lack of reliable probing methods. Herein, we report a universally applicable approach to investigating electrocatalytic reactions at electrode/polyelectrolyte interfaces under normal electrochemical conditions. By coating a thin layer of anion-exchange membrane (AEM) onto the electrode surface, solutions with bulky organic cations were well separated, thus a pure electrode/polyelectrolyte interface can be established in a regular electrochemical setup and studied using in situ spectroscopies, e.g., attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS). We found that the blank Au surface was inert toward the CO2 reduction reaction (CO2RR) in the absence of alkali metal cations, whereas coating with an AEM can dramatically turn on the catalytic activity. ATR-SEIRAS revealed that the hydrogen bond network of water at the Au/AEM interface was enhanced in comparison to that on the blank Au surface, which facilitated the hydrogenation process of the CO2RR. These findings further our fundamental understanding of the catalytic behavior of electrode/polyelectrolyte interfaces and benefit the development of relevant electrochemical technologies.

An anti-freezing pure inorganic electrolyte for long cycle life aqueous sodium-ion batteries at -40 °C

Aqueous electrolytes have the great application potential for sodium-ion batteries owing to eco-friendliness, high-safety, and low cost. However, the high freezing point of common aqueous electrolytes greatly limits the normal operation of aqueous sodium-ion batteries (ASIBs) at low temperatures. Herein, MnCl2·4H2O is introduced into NaCl solution to form the hybrid NaCl/MnCl2·4H2O electrolyte to expand the application scope of ASIBs. Due to the strong interaction between Mn2+ and water molecules, the hydrogen bond network in water is damaged on a large scale. Thus, the hybrid electrolyte maintains a liquid state and has a high ionic conductivity (2.44 mS cm−1) at -50 °C. When used the optimized hybrid inorganic electrolyte, the pure inorganic compositions full battery assembled with Na2CoFe(CN)6 cathode and active carbon anode delivers a high specific capacity of 54.0 mAh g−1 at -40 °C under 1 C (1 C = 150 mA g−1). Excitingly, when tested at -40 °C under 10 C, the battery can achieve an ultra-long cycle stability of 10,000 cycles with a capacity retention of ∼ 99 %. Significantly, this work opens a new path to explore the ASIBs with superior electrochemical performance at low temperatures.

Diethylene glycol reduced the water activity of aqueous electrolyte via regulating interphase chemistry for highly durable Zinc-ion batteries

The uncontrollable dendrite growth and parasitic side reactions of Zn lead to poor cycling stability, hindering the practical application of aqueous zinc-ion batteries. Here, we develop a new hybrid electrolyte with zinc trifluoromethanesulfonate dissolved in water and co-solvent diethylene glycol (DEG). DEG can not only alter the Zn2+ solvation structure with the co-participation of DEG and anion to reduce active water molecules, but also interrupt the hydrogen-bond network of the original water. DEG is more easily absorbed on Zn surface than H2O to regulate electric double layer. Based on these unique effects, DEG can regulate interface chemistry, forming a robust solid electrolyte interphase and adjusting Zn2+ stripping/plating behaviors, which suppress side reactions and dendrite growth. Their synergetic effect results in the great improved cycling stability of Zn anode with 5000 h in symmetric cell at 1 mA cm−2 and 1 mAh cm−2. The work shed light on the design of high-performance aqueous electrolyte to advance zinc-ion batteries.

Hydration of N-Hydroxyurea from Ab Initio Molecular Dynamics Simulations.

N-Hydroxyurea (HU) is an important chemotherapeutic agent used as a first-line treatment in conditions such as sickle cell disease and β-thalassemia, among others. To date, its properties as a hydrated molecule in the blood plasma or cytoplasm are dramatically understudied, although they may be crucial to the binding of HU to the radical catalytic site of ribonucleotide reductase, its molecular target. The purpose of this work is the comprehensive exploration of HU hydration. The topic is studied using ab initio molecular dynamic (AIMD) simulations that apply a first principles representation of the electron density of the system. This allows for the calculation of infrared spectra, which may be decomposed spatially to better capture the spectral signatures of solute-solvent interactions. The studied molecule is found to be strongly hydrated and tightly bound to the first shell water molecules. The analysis of the distance-dependent spectra of HU shows that the E and Z conformers spectrally affect, on average, 3.4 and 2.5 of the closest H2O molecules, respectively, in spheres of radii of 3.7 Å and 3.5 Å, respectively. The distance-dependent spectra corresponding to these cutoff radii show increased absorbance in the red-shifted part of the water OH stretching vibration band, indicating local enhancement of the solvent's hydrogen bond network. The radially resolved IR spectra also demonstrate that HU effortlessly incorporates into the hydrogen bond network of water and has an enhancing effect on this network. Metadynamics simulations based on AIMD methodology provide a picture of the conformational equilibria of HU in solution. Contrary to previous investigations of an isolated HU molecule in the gas phase, the Z conformer of HU is found here to be more stable by 17.4 kJ·mol-1 than the E conformer, pointing at the crucial role that hydration plays in determining the conformational stability of solutes. The potential energy surface for the OH group rotation in HU indicates that there is no intramolecular hydrogen bond in Z-HU in water, in stark contrast to the isolated solute in the gas phase. Instead, the preferred orientation of the hydroxyl group is perpendicular to the molecular plane of the solute. In view of the known chaotropic effect of urea and its N-alkyl-substituted derivatives, N-hydroxyurea emerges as a unique urea derivative that exhibits a kosmotropic ordering of nearby water. This property may be of crucial importance for its binding to the catalytic site of ribonucleotide reductase with a concomitant displacement of a water molecule.

Why does urea not alter the vibrational spectroscopic signatures of water?

Usually, external solutes alter the local structural arrangement of the water hydrogen bond (H-bond) network. However, urea has a negligible effect on the local structure of water, irrespective of its concentration. In this work, we aim to find the microscopic origin of the inertness of urea toward water’s local structure by using theoretical isotope dilute IR spectroscopy. To get a microscopic resolution of different local environments, we investigate frequency distributions, population of structurally different ensembles, H-bond configurations, and H-bond strength. We find that urea has a negligible effect on the vibrational spectroscopic signatures of water. The solvation shell-wise decomposition of frequency distribution further reveals that the urea has almost zero perturbation to the local structure of any of its solvation shells. However, the frequency distribution of waters near the C=O group and NH2 group reveals a non-negligible impact by urea on water. The frequency distribution of the CO-region is red-shifted and narrower than the bulk water response, indicating a stronger H-bond and enhanced structural ordering of the waters in the CO-region; however, an opposite response is observed for the NH-region. The H-bond strength outcome further supplements this finding. We infer that the O-H oscillators in the CO-region and NH-region have non-negligible counteracting perturbation from the urea molecule. Yet, the overall response is free from any such effects. The insignificant populations and counteracting responses of these two ensembles play a major role.

Alkali hydroxide (LiOH, NaOH, KOH) in water: Structural and vibrational properties, including neutron scattering results.

Structural and vibrational properties of aqueous solutions of alkali hydroxides (LiOH, NaOH, and KOH) are computed using quantum molecular dynamics simulations for solute concentrations ranging between 1 and 10M. Element-resolved partial radial distribution functions, neutron and x-ray structure factors, and angular distribution functions are computed for the three hydroxide solutions as a function of concentration. The vibrational spectra and frequency-dependent conductivity are computed from the Fourier transforms of velocity autocorrelation and current autocorrelation functions. Our results for the structure are validated with the available neutron data for 17M concentration of NaOH in water [Semrouni et al., Phys. Chem. Chem. Phys. 21, 6828 (2019)]. We found that the larger ionic radius [rLi+<rNa+<rK+] and higher concentration disturb the hydrogen-bond network of water, resulting in more disordered cationic hydration shell. Our abinitio simulation data for solute concentrations ranging between 1 and 10M can be used to guide future elastic and inelastic neutron-scattering experiments.