Network Structure Of Water Research Articles

Entropy Changes in Water Networks Promote Protein Denaturation.

For over a century, an explanation for how concentrated ions denature proteins has proven elusive. Here, we report a novel mechanism of protein denaturation driven by entropy changes in water networks. Experiments and simulations show that ion pairs like LiBr and LiCl localize water molecules and disrupt the water network's structure, while others exert a more global effect without compromising network integrity. This disruption reduces the entropy penalty when proteins sequester water molecules during unfolding, resulting in a peculiar yet universal "inverse hydrophobic effect" that potentiates protein denaturation. Through successful isolation and systematic study of indirect solute effects, our findings offer a universal approach to salt induced protein denaturation and provide a unified framework for the decoding of the protein-water-solute nexus.

Layered V10O24·nH2O as a new ammonium ion host material for aqueous and quasi-solid-state ammonium-ion hybrid capacitors

Aqueous ammonium-ion hybrid capacitors (AIHCs) emerge as a promising candidate for efficient and sustainable charge storage. Yet, a pivotal challenge lies in the development of an ammonium ion (NH4+) host material that possesses high capacity and prolonged cycle life. Herein, we explore the potential of layered V10O24·nH2O, synthesized via electrodeposition method, for use in high-capacity aqueous NH4+ storage. Our investigation, supported by both experimental observations and first-principles theoretical computations, has demonstrated that the layered V10O24·nH2O exhibits commendable electrochemical performance for aqueous NH4+ storage, which is attributed to the presence of certain amount of crystal water and unique nanowire network structure. This allows for a high specific capacity of 203.1 mAh g−1 at 0.3 A g−1, and the capacity retention is 97.6 % after 20,000 cycles. Ex-situ characterizations uncovered that the insertion and extraction of NH4+ in the V10O24·nH2O layers are reversible processes, accompanied by changes in the oxidation states of vanadium and the reversible contraction and expansion of the interlayer spacing. Furthermore, the as-assembled AIHCs device not only exhibits a voltage window of 1.8 V, surpassing other types of hybrid capacitors, but also retains 82.8 % capacitance after 10,000 cycles, showcasing its good flexibility and potential for series–parallel combinations. The study highlights the potential of layered V10O24·nH2O electrodes for sustainable energy storage applications and offers some insights for high-performance hybrid capacitors with non-metallic NH4+ as the charge carrier.

X-ray diffraction and quasielastic neutron scattering studies of the structure and dynamic properties of water confined in ordered microporous carbon pores

The structure and dynamic properties of capillary-condensed water confined in ordered microporous carbon (OMC) of pores diameter 18.7 Å are investigated over a temperature range of 200–300 K by adsorption/desorption isotherms, X-ray diffraction (XRD), and quasielastic neutron scattering (QENS). The nitrogen adsorption/desorption isotherm of OMC pores at 77 K exhibits an I-type pattern. The water adsorption/desorption isotherm of OMC pores at 298 K is of type V. The XRD data on water confined in OMC reveal that the tetrahedral network structure of water is perturbed from the bulk water structure, but not to such an extent as found for water confined in MCM-41 and Ph-PMO previously reported. With decreasing the temperature, the ∼2.8 Å peak shifts to shorter distances, while the second-neighbor H2O– H2O interaction distances gradually increase from 3.95 Å and 4.49 Å to 4.43 Å and 4.84 Å, indicating a tendency to form a more tetrahedral-like hydrogen-bonded water structure at subzero temperatures. Below 230 K, the hexagonal ice Ih was partially formed in OMC pores. The QENS spectra were analyzed using a jump-diffusion model to translate water molecules. The translational diffusion of water molecules in OMC pores is comparable to that of bulk water at 300 K and higher than that in MCM-41, and the mobility slows as the temperature decreases. The elastic incoherent structure factor (EISF) analysis found evidence for immobile and mobile fractions of confined water. The mobile fraction exhibited jump diffusion, with a jump length consistent with a sphere of confinement radius of 4–8 Å. The results obtained in the present work are compared with those reported for MCM-41 with a hydrophilic interface and Ph-PMO with an amphiphilic interface, and the influence of interface effect on local structure and dynamic properties of confined water is discussed.

Effect of salt and alkali on the viscoelastic behavior of noodle dough sheet with different wheat starch granule sizes

The underlying mechanisms of salt and alkali on the viscoelastic behaviors of noodle dough sheets with varied B/A-type starch ratios were investigated from water state, protein polymerization and conformation, and microstructure. The viscoelastic behaviors of dough sheets increased with increasing B/A-type starch ratio, regardless of the presence of salt and alkali, indicating the addition of salt and alkali did not change the effect law of starch granule size on dough viscoelasticity. The viscoelastic moduli of dough decreased in the presence of salt and alkali, and the effect was more obvious as the ratio of B/A-type starch decreased, which was mainly determined by the interactions of protein-protein, protein-starch, and starch-starch in dough systems. In the low ratio of B/A-type starch dough sheets, NaCl enhanced the non-covalent interactions and β-sheet structure, while alkali promoted the covalent cross-linking of protein. In the high ratio B/A-type starch dough samples, the big starch surface area provided by a high phase volume of starch granules led to the domination of starch-starch interactions over the protein phase, thus determining the viscoelastic behavior of dough. SEM images showed that NaCl caused the gluten to form a fibrous structure, while alkali induced a membrane-like and more closed structure. NaCl and alkali showed different influences on water distribution, molecular conformation, and network structure of dough sheets with varied B/A-type starch ratios and thus contributed to the different viscoelastic behaviors.

Effect of ion-specific water structures at metal surfaces on hydrogen production

Water structures at electrolyte/electrode interfaces play a crucial role in determining the selectivity and kinetics of electrochemical reactions. Despite extensive experimental and theoretical efforts, atomic-level details of ion-specific water structures on metal surfaces remain unclear. Here we show, using scanning tunneling microscopy and noncontact atomic force microscopy, that we can visualize water layers containing alkali metal cations on a charged Au(111) surface with atomic resolution. Our results reveal that Li+ cations are elevated from the surface, facilitating the formation of an ice-like water layer between the Li+ cations and the surface. In contrast, K+ and Cs+ cations are in direct contact with the surface. We observe that the water network structure transitions from a hexagonal arrangement with Li+ to a distorted hydrogen-bonding configuration with Cs+. These observations are consistent with surface-enhanced infrared absorption spectroscopy data and suggest that alkali metal cations significantly impact hydrogen evolution reaction kinetics and efficiency. Our findings provide insights into ion-specific water structures on metal surfaces and underscore the critical role of spectator ions in electrochemical processes.

Uncovering the structure and evolution of global virtual water and agricultural land network

The effective management and allocation of water and land resources is pivotal for ensuring global food security and facilitating the transition towards sustainable development. Combining multi-regional input-output analysis and complex network modelling, this study examining the spatial-temporal evolution and topological structures of multi-layer virtual water and agricultural land networks, analyzed the network characteristics of different countries/regions, and tested the network vulnerability between virtual water trade network and virtual agricultural land network. From the results, it is revealed that 30.9 %—34.14 % of global water resources and 32.9 %—40 % of global agricultural land are associated with international trade. Meanwhile, the geographical distribution of this trade has shifted from low-income countries to middle and high-income countries, showing three distinct fluctuations in their instability levels. Additionally, quantitative network analysis indicates that resource trade networks exhibit small-world characteristics with increasing trends in network density, clustering coefficient, and average path length values over time. Among the two disturbance scenarios, both virtual water and virtual agricultural land networks were more vulnerable under deliberate assault than under random failure, however, the agricultural land network demonstrates greater toughness compared to the virtual water network. These findings highlight the importance of sustainably managing global water and land resources within a framework for sustainable development which aims at promoting both worldwide food security and environmental protection simultaneously.

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.

Synergistic M‐O Dual‐Atom Pairs Induced Interfacial Water Hydrogen Bonding Network for Boosting MoSe2 Electrocatalytic Performance

AbstractUnderstanding the dynamics changes of the water network at the electrode–solution interface during the hydrogen evolution reaction (HER) process, including how it is doubly regulated by the electrode material and electrolyte pH, and its subsequent effects on the reaction intermediates (H* and OH*), is crucial in electrochemistry. However, relevant studies are limited due to water's its dual role as both a reactant and a solvent. Thus, it is essential to construct an ideal model capable of decoupling the effects of interfacial water action from the surface catalytic HER process. In this study, M‐O atom pairs doped MoSe2 model catalyst is developed to achieve this goal and tailor the water network structure in a double‐layer microenvironment. Combined with molecular dynamics simulations and in situ spectroscopic characterization, correlations between water configuration, the water network, and water dissociation with HER activity are successfully established. This findings reveal that the pH‐dependent hydrogen‐bonding environment, modulated by oxophilic species, exerts a greater influence on acidic HER compared to alkaline media. The optimized Rh,O‐MoSe2‐x catalyst demonstrates exceptional performance in both acid and alkaline electrolytes and shows no activity decay during a PEMWE test at 1.5 A cm−2, making it promising for scalable water electrolyzers.

Impacts of the Middle Route of China's South-to-North Water Diversion Project on the water network structure in the receiving basin.

The Middle Route of South-to-North Water Diversion Project (MRSNWD) is the main skeleton of China's National Water Network, its construction has changed the structure of the original water network, and analyzing the topological change of the water network in context with MRSNWD is significant for water network planning and management. In this study, the overall network characteristics of the water network in 2010 and 2020 were analyzed based on the small-world and scale-free characteristics of complex network theory. The topological changes of the water network from a node perspective were examined using three network centrality indexes: degree centrality (DC), closeness centrality (CC), and betweenness centrality (BC), while assessing the important nodes of the water network and recognizing functional areas of cold-hot spots. The results show that the water network's centrality in the study area improved after the project construction, with the average degree of the water network increasing from 2.39 to 2.42 and the average path length decreasing from 111.81 to 97.08. The propagation efficiency and network stability also increased, with a rise in important node proportion from 9.8 to 14.4%. The nodes in the DC hotspot zone along the project route have increased by 1.5%, implying an increase in the connectivity of the water network, while MRSNWD optimizes its north-south hub propagation path. "Small-worldness" indicates that most nodes of a network can be accessed and connected over shorter paths. The water network has a significant "small-worldness" and has been enhanced by the MRSNWD's construction. Approximating the water network as a scale-free network can impact its security by identifying critical nodes. The results of this research can provide the necessary technical support and reference significance for China's National Water Network.

The Impact of Large-Scale Water Diversion Projects on the Water Supply Network: A Case Study in Southwest China

The uneven spatial and temporal distribution of water resources has consistently been one of the most significant limiting factors for social development in many regions. Furthermore, with the intensification of climate change, this inequality is progressively widening, posing a critical challenge to the sustainable development of human societies. The construction of large-scale water projects has become one of the crucial means to address the contradictions between water supply and demand. Thus, evaluating the functional aspects of water source network structures and systematically planning the layout of engineering measures in a scientifically reasonable manner are pressing issues that require urgent attention in current research efforts. Addressing this, our study takes the Erhai Lake basin and the surrounding areas in southwest China as the study area and combines landscape ecology and network analysis theory methods to propose a water supply network analysis method that takes into account both structure and node characteristics. Based on this methodology, we analyze the connectivity characteristics of water supply networks in the Erhai region under current (2020) and future (2035) planning scenarios. The results show that there were 215 nodes and 216 links in the water supply network of the Erhai Lake basin in 2020; with the implementation of a series of water conservancy projects, the planned 2035 water supply network will increase by 122 nodes and 163 links, and the connectivity of the regional water network will be significantly improved. Also, we identify some key nodes in the network, and the results show that the water supply network in 2035 will have obvious decentralization characteristics compared with that in 2020. And, based on the network degradation analysis, we find that with the implementation of engineering measures, the resilience of the water supply network will be significantly strengthened by 2035, with stronger risk tolerance. This study extends the quantitative representation of water source network characteristics, which can provide a useful reference for water network structure planning and optimization.

Effects of Hydrogen Peroxide on the Hydrogen Bonding Structure and Dynamics of Water and Its Influence on the Aqueous Solvation of the Insulin Monomer.

The hydrogen bond structure and dynamics of water and hydrogen peroxide (H2O2) in their binary mixtures have been studied at 298 K by classical molecular dynamics simulations. Twelve different concentrations of aqueous-H2O2 solutions are considered for this study. We have analyzed the interactions between water and H2O2 by site-site pair correlation functions and observed that the probability of formation of OW···HP hydrogen bonds are higher compared to OP···HW. The second solvation shell of water is strongly affected by increasing H2O2 concentrations (XP > 0.50), which signifies the destruction of the tetrahedral network structure of water. The translational and rotational dynamics of water and H2O2 do not significantly change up to 25% of H2O2 in aqueous mixtures. The hydrogen bond lifetime of water-water, water-H2O2, and H2O2-H2O2 in the aqueous-H2O2 solutions shows a very minimal change with increasing H2O2 concentrations. In addition to this, we also investigated the effect of H2O2 on the insulin monomer and observed that higher concentrations of H2O2 (XP = 0.10) change the secondary structure. The influence of H2O2 is more on chain-B than that on chain-A in the insulin monomer. The H2O2 occupancy at the protein surface is higher for negatively charged (GLU) and polar (ASN and THR) amino acid residues compared with that for positively charged and neutral residues in the solutions.

Copper coordination polymer with lattice water molecules and strong electrocatalytic OER activity

The versatility of organic ligand and metal coordination geometry produced coordination polymer with intriguing network structure and exciting functional properties. Herein, we have synthesized a copper coordination polymer (Cu-HS) using an amino acid based multidentate ligand and explored its electrocatalytic OER activity in alkaline condition. Single crystal structural studies showed the formation of 1D coordination network structure and inclusion of lattice water. Copper ions in Cu-HS displayed octahedral and square pyramidal coordination geometry. Electrocatalytic OER studies in alkaline medium showed strongly enhanced activity for Cu-HS polymer that required an overpotential of 273 mV to achieve the benchmark current density of 10 mA/cm2. Tafel slope analysis and electrochemical impedance studies suggested faster reaction kinetics at the electrode surface modified using Cu-HS. After catalysis, XPS and FTIR spectra of Cu-HS suggested the conversion to metal oxide during the electrocatalysis.

Rapid Kinetic Interactions of Sugar and Sugar Alcohol with Sweet Taste Receptors on Live Cells Using Stopped-Flow Spectroscopy.

The subjective measurement of the dynamic perception of sweetness is a problem in food science. Herein, the rapid interactions of sugars and sugar alcohols with sweet taste receptors on living cells on a millisecond timescale were studied via stopped-flow fluorescence spectroscopy. According to the rapid-kinetic parameters, sweeteners were divided into two groups. Sweeteners in group I disrupted the hydrogen bond network structure of water, and the apparent rate constant (kobs) was in the range of 0.45-0.6 s-1. Sweeteners in group II promoted the hydrogen bond formation of water, and the kobs was mostly in the range of 0.6-0.75 s-1. For most sweeteners, the kobs of cell responses was negatively correlated with the apparent specific volume of sweeteners. The differences in the cellular responses may be attributed to the disturbance in the water structure. Experimental results showed that the kinetic parameters of sweet cell responses reflected the dynamic perception of sweetness. Rapid kinetics, solution thermodynamic analysis, and water structure analysis enriched the physicochemical study of the sweetness mechanism and can be used to objectively evaluate the dynamic perception of sweetness.

Interprovincial Virtual Water-Energy Flow and Its Network Structure Resilience in Yangtze River Economic Belt

Water and energy are essential resources that flow between different regions in economic activities, forming a complex network that profoundly impacts sustainable development. Revealing network structural resilience allows for the identification of weak links, thus enhancing the capacity for sustainable development. This study employs a resilience-based method to examine changes in virtual water-energy transfers, combining input–output tables and total resource consumption coefficients (TRCC) to investigate the structural resilience of the virtual water-energy network. Case studies were conducted in the Yangtze River Economic Belt (YEB) in 2012 and 2017. The results show that the virtual water flow rate decreased by 28.66%, while that of virtual energy increased by 4.88% in YEB. The virtual energy network’s structural resilience is better than that of the virtual water network and shows significant improvement in later periods. The virtual water network structure has a clear hierarchical structure, while the virtual energy network structure is relatively flat. The transmission and connectivity of the two networks do not differ significantly, but the virtual energy network’s transmission is superior to that of the virtual water network. There is a significant improvement in the virtual energy network’s agglomeration in the later stages, while there is no significant change in the virtual water contact network.

Understanding the Effect of Single Atom Cationic Defect Sites in an Al2O3 (012) Surface on Altering Selenate and Sulfate Adsorption: An Ab Initio Study.

Adsorption is a promising under-the-sink selenate remediation technique for distributed water systems. Recently it was shown that adsorption induced water network re-arraignment control adsorption energetics on the (012) surface. Here, we aim to elucidate the relative importance of the water network effects and surface cation identity on controlling selenate and sulfate adsorption energy using density functional theory calculations. Density functional theory (DFT) calculations predicted the adsorption energies of selenate and sulfate on nine transition metal cations (Sc-Cu) and two alkali metal cations (Ga and In) in the (012) surface under simulated acidic and neutral pH conditions. We find that the water network effects had larger impact on the adsorption energy than the cationic identity. However, cation identity secondarily controlled adsorption. Most cations decreased the adsorption energy weakening the overall performance, the larger Sc and In cations enabled inner-sphere adsorption in acidic conditions because they relaxed outward from the surface providing more space for adsorption. Additionally, only Ti induced Se selectivity over S by reducing the adsorbing selenate to selenite but not reducing the sulfate. Overall, this study indicates that tuning water network structure will likely have a larger impact than tuning cation-selenate interactions for increasing adsorbate effectiveness.

Pollution in river tributaries restricts the water quality of ecological water replenishment in the Baiyangdian watershed, China.

Natural rivers often have complex water network structures, and the continuous water inflow from tributaries may have crucial impacts on the water quality of ecological water replenishment in the mainstream. This study selected two main inflow rivers of the largest lake in Hebei Province (Baiyangdian), the Fu River and Baigou River, to explore the influence of tributaries on the quality changes of ecological replenishment water in the mainstreams. In December 2020 and 2021, water samples were collected along the two river routes, and eutrophic parameters and heavy metals were determined. The results showed that the tributaries of the Fu River were all severely polluted. With the inflows of the tributaries, the comprehensive pollution index of eutrophication greatly increased along the replenished water route of the Fu River, and the replenished water in the lower reaches of the Fu River mainstream was mostly considered moderate to heavy pollution. Whereas, because the Baigou River's tributaries were only moderately polluted, the water quality in the Baigou River's replenished water was mostly better than moderate pollution. Due to the slight pollution of heavy metals in the tributaries, the replenished water in both the Fu and Baigou Rivers did not show any impact from heavy metal pollution. Correlation and principal component analysis indicated that the main sources of serious eutrophic pollution in the tributaries of the Fu and Baigou Rivers were related to domestic sewage, industrial wastewater, plant decay, and sediment release. This non-point source pollution then caused the decline in the quality of the replenished water in the mainstreams. This study exposed a long-standing but neglected problem in ecological water replenishment and provided a scientific foundation for conducting better water management to improve the inland water environment.

Structural analysis of water networks

AbstractLiquid water, besides being fundamental for life on Earth, has long fascinated scientists due to several anomalies. Different hypotheses have been put forward to explain these peculiarities. The most accredited one foresees the presence in the supercooled region of two phases at different densities: the low-density liquid phase and the high-density liquid phase. In our previous work [Faccio et al. (2022), J. Mol. Liq., 355, 118922], we showed that it is possible to identify these two forms in water networks through a computational approach based on molecular dynamics simulation and on the calculation of the total communicability of the associated graph, in which the nodes correspond to water molecules and the edges represent the connections (interactions) between molecules. In this article, we present a more in-depth investigation of the application of graph-theory based approaches to the analysis of the structure of water networks. In particular, we investigate different connectivity and centrality measures and we report on the use of a variety of global metrics aimed at giving a topological and geometrical characterization of liquid water.

Revealing the impact of a water-economy nexus-based joint tax management policy on the environ-economic system: An advanced exploration of double dividend strategies and multi-scale response mechanisms

Economic growth is constrained by water scarcity, and a unified policy analysis framework is required to enhance the coordinated development of the environ-economic system from the perspective of wastewater management. Thus, a multi-scale water-economic double dividend mechanism model (MWED) is first developed to (i) derive strategies for simultaneously achieving water scarcity mitigation and economic increase through compounding wastewater tax (WT) policies and reduced value-added tax (RVT) policies; (ii) explore the internal response mechanisms at the sectoral scale in the central region; and (iii) reveal the responses of economic output and multiple water resources in external regions under the cascading effects. This integrated approach of a computable general equilibrium model, an ecological network analysis, and a multi-regional input-output analysis is applied to Shanxi Province, China, a representative water-scarce region. The double dividend strategies of WT_6 yuan/ton*RVT_2%, WT_8 yuan/ton*RVT_2.5%, and WT_10 yuan/ton*RVT_3% were conducive to alleviating water scarcity and stimulating economic growth by adjusting the production structures or upgrading treatment technologies to reduce wastewater discharge, reducing the use of water-intensive energy sources to condense direct water consumption, and enhancing the connection between low water consumption sectors and advantageous economic sectors to optimize the virtual water network structure. Based on complex inter-regional relationships, these cascading effects can stimulate the economic output of other provinces and alleviate prevailing water scarcities by increasing virtual water inflows in economically developed regions and decreasing direct water consumption in economically undeveloped regions. The ability of water-rich regions to reconcile differences in water resource endowments can be further strengthened.

A subtle interplay between hydrophilic and hydrophobic hydration governs butanol (de)mixing in water

A possible molecular origin of the contorting water-solubility of butanol isomers lies in the self-association propensity of alcohols as well as on the specific interaction between the hydrophilic and hydrophobic moiety of butanol(s) with water. We have made a synergistic approach using far-IR (50–600 cm−1)-FTIR and MD simulation measurements to probe the extent of alteration of HBond structure of water-network in water-alcohol mixtures.The experimental and computational observations infer that extent of hydration of the non-polar moiety of the alcohol self-aggregates plays a decisive role in the (de)mixing of butanol(s) in water.

Construction of a decellularized spinal cord matrix/GelMA composite scaffold and its effects on neuronal differentiation of neural stem cells

Spinal cord injury (SCI) leads to severe loss of motor and sensory functions, and the rehabilitation of SCI is a worldwide problem. Tissue-engineered scaffolds offer new hope for SCI patients, while the newly developed materials encountered a challenge in modeling the microenvironment around the lesion site. We constructed a new composite scaffold by mixing decellularized spinal cord extracellular matrix (dECM) with gelatin methacryloyl (GelMA). The dECM, as a natural biological material, retained a large number of proteins and growth factors related to neurogenesis. GelMA was a photopolymerizable material, harbored a polymer network structure, soft texture, certain shape and plenty of water. The viability, proliferation, and differentiation of neural stem cells (NSCs) on the composite scaffold were evaluated by cell count kit-8 (CCK8), Live/Dead assay, phalloidin staining, 5-Ethynyl-2’-deoxyurdine (EdU), immunofluorescence staining and western blot. The Live/Dead assay, phalloidin staining, EdU, and CCK8 assay showed that the composite scaffold had good biocompatibility and provided better support for proliferation of NSCs. Results of immunocytochemistry and western blot showed that the composite scaffolds promoted the specific differentiation of NSCs into neuron cells. Together, this dECM/GelMA composite scaffold can be used as a cell culture coating, the isolated NSCs seeded on the surface of composite scaffold expressed neuronal markers and assumed neuronal morphology. Our work provided a new method that would be widely used in tissue engineering of SCI.