Macromolecular crowding potently stimulates DNA supercoiling activity of Mycobacterium tuberculosis DNA gyrase.

Macromolecular crowding, manifested by high concentrations of proteins and nucleic acids in living cells, significantly influences biological processes such as enzymatic reactions. Studying these reactions in vitro, using agents such as polyetthylene glycols (PEGs) and polyvinyl alcohols (PVAs) to mimic intracellular crowding conditions, is essential due to the notable differences from enzyme behaviors observed in diluted aqueous solutions. In this article, we studied Mycobacterium tuberculosis (Mtb) DNA gyrase under macromolecular crowding conditions by incorporating PEGs and PVAs into the DNA supercoiling reactions. We discovered that high concentrations of potassium glutamate, glycine betaine, PEGs, and PVA substantially stimulated the DNA supercoiling activity of Mtb DNA gyrase. Steady-state kinetic studies showed that glycine betaine and PEG400 significantly reduced the KM of Mtb DNA gyrase and simultaneously increased the Vmax or kcat of Mtb DNA gyrase for ATP and the plasmid DNA molecule. Molecular dynamics simulation studies demonstrated that PEG molecules kept the ATP lid of DNA gyrase subunit B in a closed or semiclosed conformation, which prevented ATP molecules from leaving the ATP-binding pocket of DNA gyrase subunit B. The stimulation of the DNA supercoiling activity of Mtb DNA gyrase by these molecular crowding agents likely results from a decrease in water activity and an increase in excluded volume.

Catalysis of Indium Ion Electroreduction in the Presence of Acetazolamide in Chlorates(VII) Solutions with Varied Water Activity.

The influence of acetazolamide (ACT) on the kinetics and the mechanism of electroreduction of In(III) ions as a function of changes of the water activity was investigated using electrochemical methods (DC, SWV, CV and EIS, CV). The multi-step mechanism of the electroreduction process should take into account the dehydration step of indium ions and the presence of In-ACT (,,cap-pair" effect) active complexes, mediating electron transfer, located in the adsorption layer. Differences in the electrode mechanism in the presence of ACT were observed for higher chlorates(VII) concentrations (above 4 mol ⋅ dm-3 chlorates(VII)) reflected by a lack of step wise nature of the electrode process. The highest catalytic activity was observed in 4 mol ⋅ dm-3 chlorates(VII).

A Mathematical Model of Diel Activity and Long Time Survival in Phototrophic Mixed-Species Subaerial Biofilms.

Subaerial biofilms (SAB) are intricate microbial communities living on terrestrial surfaces, of interest in a variety of contexts including cultural heritage preservation, microbial ecology, biogeochemical cycling, and biotechnology. Here we propose a mathematical model aimed at better understanding the interplay between cyanobacteria and heterotrophic bacteria, common microbial SAB constituents, and their mutual dependence on local environmental conditions. SABs are modeled as thin mixed biofilm-liquid water layers sitting on stone. A system of ordinary differential equations regulates the dynamics of key SAB components: cyanobacteria, heterotrophs, polysaccharides and decayed biomass, as well as cellular levels of organic carbon, nitrogen and energy. These components are interconnected through a network of energetically dominant metabolic pathways, modeled with limitation terms reflecting the impact of biotic and abiotic factors. Daily cylces of temperature, humidity, and light intensity are considered as input model variables that regulate microbial activity by influencing water availability and metabolic kinetics. Relevant physico-chemical processes, including pH regulation, further contribute to a description of the SAB ecology. Numerical simulations explore the dynamics of SABs in a real-world context, revealing distinct daily activity periods shaped by water activity and light availability, as well as longer time scale survivability conditions. Results also suggest that heterotrophs could play a substantial role in decomposing non-volatile carbon compounds and regulating pH, thus influencing the overall composition and stability of the biofilm.

A meta-analysis of microbial thermal inactivation in low moisture foods.

Microbial thermal inactivation in low moisture foods is challenging due to enhanced thermal resistance of microbes and low thermal conductivity of food matrices. In this study, we leveraged the body of previous work on this topic to model key experimental features that determine microbial thermal inactivation in low moisture foods. We identified 27 studies which contained 782 mean D-values and developed linear mixed-effect models to assess the effect of microorganism type, matrix structure and composition, water activity, temperature, and inoculation and recovery methods on cell death kinetics. Intraclass correlation statistics (I2) and conditional R2 values of the linear mixed effects models were: E. coli (R2-0.91, I2-83%), fungi (R2-0.88, I2-85%), L. monocytogenes (R2-0.84, I2-75%), Salmonella (R2-0.69, I2-46%). Finally, global response surface models (RSM) were developed to further study the non-linear effect of aw and temperature on inactivation. The fit of these models varied by organisms from R2 0.88 (E. coli) to 0.35 (fungi). Further dividing the Salmonella data into individual RSM models based on matrix structure improved model fit to R2 0.90 (paste-like products) and 0.48 (powder-like products). This indicates a negative relationship between data diversity and model performance.

How the interplay of molecular and colloidal scales controls drying of microgel dispersions.

Bringing an aqueous dispersion or solution into open air leads to water evaporation. The resulting drying process initiates the buildup of spatial heterogeneities, as nonvolatile solutes and colloids concentrate. Such composition gradients associate with mesostructure gradients, which, in turn, impact flows within these multicomponent systems. In this work, we investigate the drying of microgel dispersions in respect to two reference systems, a colloidal dispersion and a polymer solution, which, respectively, involve colloidal and molecular length scales. We evidence an intermediate behavior in which a film forms at the air/liquid interface and is clearly separated from bulk by a sharp drying front. However, complex composition and mesostructure gradients develop throughout the drying film, as evidenced by Raman and small-angle X-ray scattering mapping. We show that this results from the soft colloidal structure of microgel, which allows them to interpenetrate, deform, and deswell. As a result, water activity and water transport are drastically decreased in the vicinity of the air/liquid interface. This notably leads to diffusional drying kinetics that are nearly independent on the air relative humidity. The interplay between water fraction, water activity, and mesostructure on water transport is generic and, thus, shown to be pivotal in order to master evaporation in drying complex fluids.

Water thermodynamics and lipid oxidation in stored whey butter.

Whey butter is the result of the rational use of the whey component, which is cream whey. It is an alternative to milk cream butter. The aim of the presented study was to analyze the effect of storage conditions on water thermodynamics and cholesterol oxidation products as reliable markers of quality and safety. After 4 mo of storage, the water loss (at 3°C and 13°C) and water activity in whey butter (only at 13°C) were reduced. Three-factorial ANOVA showed that the value of water activity was independent of the type of butter in interaction with the storage temperature. The duration of the translational movement of water molecules from the inside of whey butter was definitely longer than in butter and shortened with storage time. This was in contrast to butter. For whey butter stored at 13°C, the kinetics of the movement of water molecules was at the highest speed. In the case of whey butter and butter, the higher storage temperature almost doubled the gloss. Increasing the temperature to 13°C resulted in different yellowness index, chroma, and browning index between whey butter and butter. There were no statistically significant differences in the percentage of fatty acids and triacylglycerols in whey butter and milk cream butter during storage. In whey butter, compared with butter, the cholesterol content was higher, but the amount of cholesterol oxidation products was smaller. However, in whey butter, these amounts increased significantly. The presence of epoxides and their transformation products (i.e., triol cholesterol) was found in storage whey butter.

Effects Provided by Sugar Substitutes upon the Quality Indicators of Model Systems of Sweetened Condensed Milk in Storage.

Sweetened condensed milk (SCM) is a product widely used by both consumers and other food production branches. However, it contains a lot of sucrose. This study aimed to examine the effects provided by sugar substitutes, such as trehalose, isomaltulose, and polydextrose, upon the SCM sensory profile and valuable quality indicators, such as water activity, viscosity, acidity, crystals size, and Maillard reaction potential (browning index, color change, loss of free amino acids). The study was performed by making model systems of SCM (MSCMs) using the method of reconstitution of powdered ingredients. All the presented carbohydrate compositions in MSCMs provided Aw value typical of intermediate-moisture food, which contributes to the long-term shelf-life of the product. However, only 2 MSCMs with compositions consisted of isomaltulose, trehalose (22.55% and 22.55%); trehalose (28.19%), sucrose (5.64%), polydextrose (5.64%), isomaltulose (5.64%) showed the stability of Aw within 14-d storage period. Trehalose and polydextrose in MSCMs with mono-carbohydrate added fraction demonstrated their high structure-forming ability expressed in high values of dynamic viscosity (>30 Pa·s), provided not by crystallization. MSCMs containing trehalose in predominant amount in the carbohydrate compositions (≥50%) showed lower average crystal size (<16 µm) compared with other MSCMs with di- and tetra-carbohydrate added fractions with predominant amount of isomaltulose and polydextrose. Isomaltulose and polydextrose added to MSCMs led to pronounced browning, while trehalose and sucrose reduced this effect in MSCMs with di- and tetra-carbohydrate added fractions. Addition of 22.55% of polydextrose to carbohydrate fraction of MSCMs caused bitterness, while 5.64% didn't affect the taste. Based on the results of all the research conducted the most optimal carbohydrate compositions to produce SCM with lower calorie, sucrose contents and stable adequate values of processing and sensory properties were trehalose (22.55%) with isomaltulose (22.55%) and trehalose (28.19%) with sucrose (5.64%), polydextrose (5.64%), isomaltulose (5.64%).

Heat Resistance, Virulence, and Gene Expression of Desiccation-Adapted Salmonella Enteritidis During Long-Term Storage in Low-Water Activity Foods.

Desiccation stress could induce crossprotection and even affect virulence of Salmonella enterica. However, the influence of food matrices with low-water activity on desiccation adaptation of Salmonella still remains unclear. This study investigated the survival and adaptation of Salmonella Enteritidis in skim milk powder, ginger powder, and chocolate powder under desiccation storage conditions for a total of 12 weeks. High survival rates of Salmonella Enteritidis in all food matrices maintained over the long-term desiccation storage. Desiccation-adapted Salmonella Enteritidis enhanced heat resistance (p < 0.05) with the increase of storage time. Food composition plays an important role in the induction of crossresistance of desiccation-adapted Salmonella. After desiccation storage, Salmonella Enteritidis in ginger powder was most tolerant to heat treatment. Salmonella Enteritidis in skim milk powder was most resistant to the gastrointestinal simulation environment, and had strongest adhesion to Caco-2 cells. The effects of food composition on gene expression (rpoS, proV, otsA, otsB, grpE, dnaK, rpoH, and sigDE) in desiccation-adapted Salmonella Enteritidis were not significant (p > 0.05). At initial desiccation storage, osmotic protection-related genes (fadA, proV, otsA, and otsB), stress response regulator (rpoS), and heat-resistance-related genes (grpE, dnaK, and rpoH) were all significantly upregulated (p < 0.05). However, after 4-week storage, the expression level of desiccation-related genes, proV, otsA, otsB, grpE, dnaK, and rpoH, significantly decreased (p < 0.05). This study enables a better understanding of Salmonella's responses to long-term desiccation stress in different kinds of low-water activity foods.

Effect of Oat Fiber Preparations with Different Contents of ß-Glucan on the Formation of Acrylamide in Dietary Bread (Rusks).

In the literature, there are few reports indicating hydrocolloids as a factor capable of reducing the amount of acrylamide formed in food. Therefore, the aim of the study was to examine the ability of soluble oat fiber to reduce the amount of acrylamide formed in the process of obtaining rusks. The effect of the concentration of ß-glucans in oat fiber preparations at 20% and 30% and the amount of preparations used at 10%, 15%, and 20% was investigated. On the basis of the obtained test results, it was shown that the most optimal concentration of oat fiber preparation in rusks recipe is at 15%, regardless of the content of ß-glucan in it. This concentration makes it possible to reduce the amount of acrylamide formed in baked goods and rusks by ~70% and ~60%, respectively, while maintaining the desired physical and chemical properties of the product. In addition, it was shown that the browning index and water activity strongly correlate with the content of acrylamide in rusks, which makes them good markers of this compound in rusks. The use of hydrocolloids in the form of oat fiber preparations with different contents of ß-glucan as a tool for reducing the amount of acrylamide in rusks, at the same time, offers the possibility of enriching these products with a soluble dietary fiber with health properties.

[Effects of maltodextrin on water adsorption and thermodynamic properties of Codonopsis Radix spray-dried powder].

This study aims to reveal the effects of maltodextrin(MD) on the water adsorption and thermodynamic properties of Codonopsis Radix(DS) spray-dried powder by determining the moisture and energy changes of the powder in the process of moisture absorption. The static weighing method was used to obtain the isothermal water adsorption data of the spray-dried powder in 6 saturated salt solutions(KAc, MgCl_2·6H_2O, K_2CO_3, NaBr, NaCl, and KCl) at 3 temperatures(25, 35, and 45 ℃). Six models were used for fitting of the water adsorption process, and the most suitable model was selected based on the model performance. Furthermore, the corresponding net equivalent adsorption heat and differential entropy were calculated, and the adsorption entropy change was integrated. The linear relationship between net equivalent adsorption heat and differential entropy was drawn based on the entropy-enthalpy complementarity theory. The results showed that the water adsorption properties of DS and DS-MD spray-dried powder followed the type Ⅲ isotherm and was well fitted by the GAB model. The monolayer water content M_0 decreased with the increase in temperature. At the same temperature, the M_0 of DS spray-dried powder decreased after the addition of MD. The net equivalent adsorption heat and differential entropy of DS and DS-MD spray-dried powder decreased with the increase in water content, which presented a linear relationship. The addition of MD decreased the water activity corresponding to the lowest integral adsorption entropy of the powder, and the system became more stable. The results indicated that the spray-dried powder became more stable after the addition of MD.

Realization of Long-Life Proton Battery by Layer Intercalatable Electrolyte.

Proton batteries have attracted increasing interests because of their potential for grid-scale energy storage with high safety and great low-temperature performances. However, their development is significantly retarded by electrolyte design due to free water corrosion. Herein, we report a layer intercalatable electrolyte (LIE) by introducing trimethyl phosphate (TMP) into traditional acidic electrolyte. Different from conventional role in batteries, the presence of TMP intriguingly achieves co-intercalation of solvent molecules into the interlayer of anode materials, enabling a new working mechanism for proton reactions. The electrode corrosion was also strongly retarded with expanded electrochemical stability window. The half-cell therefore showed an outstanding long-term cycling stability with 91.0 % capacity retention at 5 A g-1 after 5000 cycles. Furthermore, the assembled full batteries can even deliver an ultra-long lifetime with a capacity retention of 74.9 % for 2 months running at -20 °C. This work provides new opportunities for electrolyte design of aqueous batteries.

Hydrated Ionic Liquids: Perspective for Bioscience.

Hydrated ionic liquid (IL) is a simple mixture of IL and water. Unique aqueous electrolyte solution can be designed by mixing IL with limited amount of water. In most hydrated ILs, there are no free water and all are strongly interacted with ions. The properties of hydrated ILs, such as polarity, viscosity, ion mobility, and hydrogen bonding ability, can therefore be controlled simply by water content. This mixture is expected to provide similar environment to that of living cell, and is desired to be effective solvents for biomolecules. In this account, we would like to survey the basic properties, recent results, and future aspects of the hydrated ILs.

Impact of sodium chloride and carbon dioxide on conidial germination and radial growth of Penicillium camemberti.

Penicillium camemberti is a domesticated species adapted to the dairy environment, which is used as adjunct cultures to ripen soft cheeses. A recent population genomics analysis on P. camemberti revealed that P. camemberti is a clonal lineage with two varieties almost identical genetically but with contrasting phenotypes in terms of growth, color, mycotoxin production and inhibition of contaminants. P. camemberti variety camemberti is found on Camembert and Brie cheeses, and P. camemberti variety caseifulvum is mainly found on other cheeses like Saint-Marcellin and Rigotte de Condrieu. This study aimed to evaluate the impact of water activity (aw) reduced by sodium chloride (NaCl) and the increase of carbon dioxide (CO2) partial pressure, on conidial germination and growth of two varieties of P. camemberti: var. Camemberti and var. Caseifulvum. Mathematical models were used to describe the responses of P. camemberti strains to both abiotic factors. The results showed that these genetically distant strains had similar responses to increase in NaCl and CO2 partial pressure. The estimated cardinal values were very close between the strains although all estimated cardinal values were significantly different (Likelihood ratio tests, pvalue = 0.05%). These results suggest that intraspecific variability could be more exacerbated during fungal growth compared with conidial germination, especially in terms of macroscopic morphology. Indeed, var. Caseifulvum seemed to be more sensitive to an increase of CO2 partial pressure, as shown by the fungal morphology, with the occurrence of irregular outgrowths, while the morphology of var. Camemberti remains circular. These data could make it possible to improve the control of fungal development as a function of salt and carbon dioxide partial pressure. These abiotic factors could serve as technological barriers to prevent spoilage and increase the shelf life of cheeses. The present data will allow more precise predictions of fungal proliferation as a function of salt and carbon dioxide partial pressure, which are significant technological hurdles in cheese production.

Genetic response of Salmonella Typhimurium to trans-cinnamaldehyde assisted heat treatment and its correlation with bacterial resistance in different low moisture food components.

Our previous study found that water activity (aw)- and matrix-dependent bacterial resistance wasdeveloped in Salmonella Typhimurium during antimicrobial-assisted heat treatment in low moisture foods (LMFs) matrices. To better understand the molecular mechanism behind the observed bacterial resistance, gene expression analysis was conducted on S. Typhimurium adapted to different conditions with or without the trans-cinnamaldehyde (CA)-assisted heat treatment via quantitative polymerase chain reaction (qPCR). Expression profiles of nine stress-related genes were analyzed. The upregulation of rpoH and dnaK and downregulation of ompC were observed during bacterial adaptation in LMF matrices and the combined heat treatment, which likely contributed to the bacterial resistance during the combined treatment. Their expression profiles were partially consistent with the previously-observed effect of aw or matrix on bacterial resistance. The upregulation of rpoE, otsB, proV, and fadA was also observed during adaptation in LMF matrices and might contribute to desiccation resistance, but likely did not contribute to bacterial resistance during the combined heat treatment. The observed upregulation of fabA and downregulation of ibpA could not be directly linked to bacterial resistance to either desiccation or the combined heat treatment. The results may assist the development of more efficient processing methods against S. Typhimurium in LMFs.

Effect of oil exposure stages on the heat resistance of Salmonella enterica serovar Enteritidis phage type 30 in peanut flour.

The oil in low-moisture foods (LMFs) shows protective effects on bacteria during thermal processing. However, the circumstances under which this protective effect strengthens remain unclear. This study aimed to understand which step of the oil exposure to bacterial cells (inoculation, isothermal inactivation, or recovery and enumeration step) in LMFs can enhance their heat resistance. Peanut flour (PF) and defatted PF (DPF) were selected as the oil-rich and oil-free LMF models. Salmonella enterica Enteritidis Phage Type 30 (S. Enteritidis) was inoculated into four designated PF groups representing different oil exposure stages. It was isothermally treated to obtain heat resistance parameters. At a constant moisture content (aw,25°C = 0.32 ± 0.02) and controlled aw,85°C (0.32 ± 0.02), S. Enteritidis exhibited significantly high (p < 0.05) D values in oil-rich sample groups. For instance, the heat resistance values of S. Enteritidis in the PF-DPF and DPF-PF groups were D80°C of 138.22 ± 7.45 min and 101.89 ± 7.82 min; however, the D80°C in the DPF-DPF group was 34.54 ± 2.07 min. The oil addition after the thermal treatment also helped injured bacterial recovery in the enumeration. For instance, the D80°C, D85°C, and D90°C values in the DFF-DPF oil groups were 36.86 ± 2.30, 20.65 ± 1.23, and 7.91 ± 0.52 min, respectively, which were higher than those in the DPF-DPF group at 34.54 ± 2.07, 17.87 ± 0.78, and 7.10 ± 0.52 min. We confirmed that the oil protected S. Enteritidis in PF in all three stages: desiccation process, heat treatment, and recovery of bacterial cells in plates.

Assessment of trans-cinnamaldehyde and eugenol assisted heat treatment against Salmonella Typhimurium in low moisture food components.

Increased thermal resistance of Salmonella at low water activity (aw) is a significant food safety concern in low-moisture foods (LMFs). We evaluated whether trans-cinnamaldehyde (CA, 1000 ppm) and eugenol (EG, 1000 ppm), which can accelerate thermal inactivation of Salmonella Typhimurium in water, can show similar effect in bacteria adapted to low aw in different LMF components. Although CA and EG significantly accelerated thermal inactivation (55 °C) of S. Typhimurium in whey protein (WP), corn starch (CS) and peanut oil (PO) at 0.9 aw, such effect was not observed in bacteria adapted to lower aw (0.4). The matrix effect on bacterial thermal resistance was observed at 0.9 aw, which was ranked as WP > PO > CS. The effect of heat treatment with CA or EG on bacterial metabolic activity was also partially dependent on the food matrix. Bacteria adapted to lower aw had lower membrane fluidity and unsaturated to saturated fatty acids ratio, suggesting that bacteria at low aw can change its membrane composition to increase its rigidity, thus increasing resistance against the combined treatments. This study demonstrates the effect of aw and food components on the antimicrobials-assisted heat treatment in LMF and provides an insight into the resistance mechanism.

Zinc Electrode Cycling in Deep Eutectic Solvent Electrolytes: An Electrochemical Study.

Among post-lithium ion battery technologies, rechargeable chemistries with Zn anodes bear notable technological promise owing to their high theoretical energy density, lower manufacturing cost, availability of raw materials and inherent safety. However, Zn anodes, when employed in aqueous electrolytes, suffer from hydrogen evolution, passivation, and shape changes. Alternative electrolytes can help tackle these issues, preserving the green and safe characteristics of aqueous-based ones. Deep eutectic solvents (DESs) are promising green and low-cost non-aqueous solvents for battery electrolytes. Specifically, the cycling of Zn anodes in DESs is expected to be reversible, chiefly owing to their dendrite-suppression capability. Nevertheless, apart from a few studies on Zn plating, insight into the cathodic-anodic electrochemistry of Zn in DESs is still very limited. In view of developing DES-based battery electrolytes, it is crucial to consider that a potential drawback might be their low ionic conductivity. Water molecules can be added to the eutectic mixtures by up to 40% to increase the diffusion coefficient of the electroactive species and lower the electrolyte viscosity without destroying the eutectic nature. In this study, we address the electrochemistry of Zn in two different hydrated DESs (ChU and ChEG with ~30% H2O). Fundamental electrokinetic and electrocrystallization studies based on cyclic voltammetry and chronoamperometry at different cathodic substrates are completed with a galvanostatic cycling test of Zn|Zn symmetric CR2032 coin cells, SEM imaging of electrodes and in situ SERS spectroscopy. This investigation concludes with the proposal of a specific DES/H2O/ZnSO4-based electrolyte that exhibits optimal functional performance, rationalized on the basis of fundamental electrochemical data, morphology evaluation and modeling of the cycling response.

Characterization of eutectic mixtures of sugars and sugar-alcohols for cryopreservation.

Natural Deep Eutectic Systems (NADES) composed of sugar and sugar alcohols have been studied and applied in a variety of biological applications. Understanding their interaction with water across dilution and temperature is inherently important for maximizing the utility of NADES. Herein a wide range of sugar:sugar-alcohol molar ratios were synthesized and characterized by viscosity, molar excess volume, differential scanning calorimetry, water activity, and confocal Raman cryomicroscopy. NADES were found to have greater viscosity, reduced heat of fusion, greater absolute molar excess volume, lower water activity, and stronger hydrogen bonding of water than non-NADES mixtures. This is hypothesized to be due to cumulatively stronger hydrogen bonding interactions between components in pure and diluted NADES with the strongest interactions in the water-rich region. This work provides useful data and further understanding of hydrogen bonding interaction strength for a wide range of molar ratios in pure to well-diluted forms.

Drying, Physical, Nutritional and Bioactive Characteristics of Apple Peel Flour Subjected to Blanching and Ultrasound Pretreatments.

The aim of this work was to study the effect of blanching and ultrasound pretreatments on drying and quality characteristics of apple peel. Blanching was conducted in boiling water, ultrasound in a water bath, and drying in a batch tray dryer. The product obtained was ground into a flour, and assessed for color, water activity, proximate composition, sugars, and bioactive compounds. Results showed that effective moisture diffusivity increases with a decrease in product moisture content, being such dependence well described by a second order polynomial model. Average drying rate was higher and product moisture content was lower for blanched and sonicated flour, especially for the former. Such result suggests that blanching and ultrasound enhance water removal during drying of apple peel. Physical properties were significantly affected by pretreatments, being more intense red color and lower water activity obtained for sonicated flour. Nutritional and bioactive properties were also significantly affected by pretreatments, being lower sugar, higher protein, fiber, catechin and epicatechin content observed for blanched flour. Summarizing, blanching and ultrasound pretreatments improve drying of apple peel, both regarding process efficiency and product quality.

A Bio-Inspired Methylation Approach to Salt-Concentrated Hydrogel Electrolytes for Long-Life Rechargeable Batteries.

Hydrogel electrolytes hold great promise in developing flexible and safe batteries, but the presence of free solvent water makes battery chemistries constrained by H2 evolution and electrode dissolution. Although maximizing salt concentration is recognized as an effective strategy to reduce water activity, the protic polymer matrices in classical hydrogels are occupied with hydrogen-bonding and barely involved in the salt dissolution, which sets limitations on realizing stable salt-concentrated environments before polymer-salt phase separation occurs. Inspired by the role of protein methylation in regulating intracellular phase separation, here we transform the "inert" protic polymer skeletons into aprotic ones through methylation modification to weaken the hydrogen-bonding, which releases free hydrogen bond acceptors as Lewis base sites to participate in cation solvation and thus assist salt dissolution. An unconventionally salt-concentrated hydrogel electrolyte reaching a salt fraction up to 44 mol % while retaining a high Na+ /H2 O molar ratio of 1.0 is achieved without phase separation. Almost all water molecules are confined in the solvation shell of Na+ with depressed activity and mobility, which addresses water-induced parasitic reactions that limit the practical rechargeability of aqueous sodium-ion batteries. The assembled Na3 V2 (PO4 )3 //NaTi2 (PO4 )3 cell maintains 82.8 % capacity after 580 cycles, which is the longest cycle life reported to date.