Thickness Measurements with EMAT Based on Fuzzy Logic.

Metal thickness measurements are essential in various industrial applications, yet current non-contact ultrasonic methods face limitations in range and accuracy, hindering the widespread adoption of electromagnetic ultrasonics. This study introduces a novel combined thickness measurement method employing fuzzy logic, with the aim of broadening the applicational scope of the EMAT. Leveraging minimal hardware, this method utilizes the short pulse time-of-flight (TOF) technique for initial thickness estimation, followed by secondary measurements guided by fuzzy logic principles. The integration of measurements from the resonance, short pulse echo, and linear frequency modulation echo extends the measurement range while enhancing accuracy. Rigorous experimental validation validates the method's effectiveness, demonstrating a measurement range of 0.3-1000.0 mm with a median error within ±0.5 mm. Outperforming traditional methods like short pulse echoes, this approach holds significant industrial potential.

Effects of molecular weight of polyaspartic acid on nitrogen use efficiency and crop yield.

BACKGROUND: In the past decades, ever-increasing fertilizer use has led to a continuous increase in agricultural output. However, serious waste of resources occurs because of the low utilization of fertilizers. Polyaspartic acid (PASP) is a biodegradable polymer that can be used as a fertilizer synergist in agricultural production to improve the nutrient utilization capacity of plants. For polymers, the molecular weight (MW) often affects their effectiveness. However, little information is available on the effects of PASP MW in agriculture, especially on nitrogen leaching and plant element uptake. RESULTS: This work was conducted to identify the effect of PASPs with three different MWs - PASP-1 (MW: 5517), PASP-2 (MW: 6934), and PASP-3 (MW: 7568) - on nitrogen leaching, lettuce growth, and wheat cultivation. The results revealed that PASP favored plant growth and nitrogen accumulation in the soil, independent of crop species. PASP with a higher MW improved yields and the agronomic characteristics of lettuce and wheat. Furthermore, apparent amelioration of nitrogen use efficiency for lettuce (7.6%, 12.8%, and 15.0%) and wheat (4.6%, 8.1%, and 9.2%) was observed in the treatments with PASP addition. The effects and merits of PASPs on preventing ammonium nitrogen leaching and improving lettuce and wheat productivity were as follows: PASP-3 > PASP-2 > PASP-1. CONCLUSION: The MW of PASP is an essential factor affecting inorganic nitrogen leaching and crop productivity, and PASP with a higher MW (7568) is recommended for application in agriculture. © 2022 Society of Chemical Industry.

Ezetimibe Increases Endogenous Cholesterol Excretion in Humans.

OBJECTIVE: Ezetimibe improves cardiovascular outcomes when added to optimum statin treatment. It lowers low-density lipoprotein cholesterol and percent intestinal cholesterol absorption, but the exact cardioprotective mechanism is unknown. We tested the hypothesis that the dominant effect of ezetimibe is to increase the reverse transport of cholesterol from rapidly mixing endogenous cholesterol pool into the stool. APPROACH AND RESULTS: In a randomized, placebo-controlled, double-blind parallel trial in 24 healthy subjects with low-density lipoprotein cholesterol 100 to 200 mg/dL, we measured cholesterol metabolism before and after a 6-week treatment period with ezetimibe 10 mg/d or placebo. Plasma cholesterol was labeled by intravenous infusion of cholesterol-d7 in a lipid emulsion and dietary cholesterol with cholesterol-d5 and sitostanol-d4 solubilized in oil. Plasma and stool samples collected during a cholesterol- and phytosterol-controlled metabolic kitchen diet were analyzed by mass spectrometry. Ezetimibe reduced intestinal cholesterol absorption efficiency 30±4.3% (SE, P<0.0001) and low-density lipoprotein cholesterol 19.8±1.9% (P=0.0001). Body cholesterol pool size was unchanged, but fecal endogenous cholesterol excretion increased 66.6±12.2% (P<0.0001) and percent cholesterol excretion from body pools into the stool increased 74.7±14.3% (P<0.0001), whereas plasma cholesterol turnover rose 26.2±3.6% (P=0.0096). Fecal bile acids were unchanged. CONCLUSIONS: Ezetimibe increased the efficiency of reverse cholesterol transport from rapidly mixing plasma and tissue pools into the stool. Further work is needed to examine the potential relation of reverse cholesterol transport and whole body cholesterol metabolism to coronary events and the treatment of atherosclerosis. CLINICAL TRIALS REGISTRATION: URL: http://www.clinicaltrials.gov. Unique identifier: NCT01603758.

Endogenous Cholesterol Excretion Is Negatively Associated With Carotid Intima-Media Thickness in Humans.

OBJECTIVE: Epidemiological studies strongly suggest that lipid factors independent of low-density lipoprotein cholesterol contribute significantly to cardiovascular disease risk. Because circulating lipoproteins comprise only a small fraction of total body cholesterol, the mobilization and excretion of cholesterol from plasma and tissue pools may be an important determinant of cardiovascular disease risk. Our hypothesis is that fecal excretion of endogenous cholesterol is protective against atherosclerosis. APPROACH AND RESULTS: Cholesterol metabolism and carotid intima-media thickness were quantitated in 86 nondiabetic adults. Plasma cholesterol was labeled by intravenous infusion of cholesterol-d7 solubilized in a lipid emulsion and dietary cholesterol by cholesterol-d5 and the nonabsorbable stool marker sitostanol-d4. Plasma and stool samples were collected while subjects consumed a cholesterol- and phytosterol-controlled metabolic kitchen diet and were analyzed by mass spectrometry. Carotid intima-media thickness was negatively correlated with fecal excretion of endogenous cholesterol (r=-0.426; P<0.0001), total cholesterol (r=-0.472; P≤0.0001), and daily percent excretion of cholesterol from the rapidly mixing cholesterol pool (r=-0.343; P=0.0012) and was positively correlated with percent cholesterol absorption (r=+0.279; P=0.0092). In a linear regression model controlling for age, sex, systolic blood pressure, hemoglobin A1c, low-density lipoprotein, high-density lipoprotein cholesterol, and statin drug use, fecal excretion of endogenous cholesterol remained significant (P=0.0008). CONCLUSIONS: Excretion of endogenous cholesterol is strongly, independently, and negatively associated with carotid intima-media thickness. The reverse cholesterol transport pathway comprising the intestine and the rapidly mixing plasma, and tissue cholesterol pool could be an unrecognized determinant of cardiovascular disease risk not reflected in circulating lipoproteins. Further work is needed to relate measures of reverse cholesterol transport to atherosclerotic disease. CLINICAL TRIAL REGISTRATION: URL: http://www.clinicaltrials.gov. Unique identifier: NCT01603758.

Preparation of intravenous cholesterol tracer using current good manufacturing practices.

Studies of human reverse cholesterol transport require intravenous infusion of cholesterol tracers. Because insoluble lipids may pose risk and because it is desirable to have consistent doses of defined composition available over many months, we investigated the manufacture of cholesterol tracer under current good manufacturing practice (CGMP) conditions appropriate for phase 1 investigation. Cholesterol tracer was prepared by sterile admixture of unlabeled cholesterol or cholesterol-d7 in ethanol with 20% Intralipid(®). The resulting material was filtered through a 1.2 micron particulate filter, stored at 4°C, and tested at time 0, 1.5, 3, 6, and 9 months for sterility, pyrogenicity, autoxidation, and particle size and aggregation. The limiting factor for stability was a rise in thiobarbituric acid-reacting substances of 9.6-fold over 9 months (P < 0.01). The emulsion was stable with the Z-average intensity-weighted mean droplet diameter remaining at 60 nm over 23 months. The zeta potential (a measure of negative surface charge protecting from aggregation) was unchanged at -36.2. Rapid cholesterol pool size was 25.3 ± 1.3 g. Intravenous cholesterol tracer was stable at 4°C for 9 months postproduction. CGMP manufacturing methods can be achieved in the academic setting and need to be considered for critical components of future metabolic studies.

Feasibility of repairing glomerular basement membrane defects in Alport syndrome.

Alport syndrome is a hereditary glomerular disease that leads to kidney failure. It is caused by mutations affecting one of three chains of the collagen α3α4α5(IV) heterotrimer, which forms the major collagen IV network of the glomerular basement membrane (GBM). In the absence of the α3α4α5(IV) network, the α1α1α2(IV) network substitutes, but it is insufficient to maintain normal kidney function. Inhibition of angiotensin-converting enzyme slows progression to kidney failure in patients with Alport syndrome but is not a cure. Restoration of the normal collagen α3α4α5(IV) network in the GBM, by either cell- or gene-based therapy, is an attractive and logical approach toward a cure, but whether or not the abnormal GBM can be repaired once it has formed and is functioning is unknown. Using a mouse model of Alport syndrome and an inducible transgene system, we found that secretion of α3α4α5(IV) heterotrimers by podocytes into a preformed, abnormal, filtering Alport GBM is effective at restoring the missing collagen IV network, slowing kidney disease progression, and extending life span. This proof-of-principle study demonstrates the plasticity of the mature GBM and validates the pursuit of therapeutic approaches aimed at normalizing the GBM to prolong kidney function.

Natural Dietary Phytosterols.

Most clinical phytosterol studies are performed by adding purified supplements to smaller phytosterol amounts present in the natural diet. However, natural dietary phytosterols themselves may also have important effects on cholesterol metabolism. Epidemiological work using food frequency questionnaires to estimate dietary intake suggest that extremes of normal consumption may be associated with 3-14% changes in LDL cholesterol. Standardized food databases do not have enough phytosterol values to allow calculation of phytosterol intake for individuals outside of specialized studies. Natural diets contain phytosterol amounts ranging from less than 60 mg/2000 kcal to over 500 mg/2000 kcal. Physiological studies in which whole body cholesterol metabolism is investigated show large effects of natural dietary phytosterols on cholesterol absorption efficiency, cholesterol biosynthesis and cholesterol excretion which exceed the magnitude of changes in LDL cholesterol. The dual effects of natural phytosterols on both LDL-C and whole body cholesterol metabolism need to be considered in relating them to potential protection from coronary heart disease risk.

Wearable Sensors Based on Miniaturized High-Performance Hybrid Nanogenerator for Medical Health Monitoring.

Wearable sensors are important components, converting mechanical vibration energy into electrical signals or other forms of output, which are widely used in healthcare, disaster warning, and transportation. However, the reliance on batteries limits the portability of wearable sensors and hinders their application in the field of Internet of Things. To solve this problem, we designed a miniaturized high-performance hybrid nanogenerator (MHP-HNG), which combined the functions of triboelectric sensing and electromagnetic power generation as well as the advantages of miniaturization. By optimizing the design of TENG and EMG, the wearable sensor achieved a voltage output of 14.14 V and a power output of 49 mW. Based on the wireless optical communication and wireless communication technologies, the wearable sensor achieved the integration of sensing, communication, and self-powered function, which is expected to realize health monitoring, emergency warning, and rehabilitation assistance, and further extend the potential application value in the medical field.

Development of Heteroatomic Constant Potential Method with Application to MXene-Based Supercapacitors.

We describe a method for modeling constant-potential charges in heteroatomic electrodes, keeping pace with the increasing complexity of electrode composition and nanostructure in electrochemical research. The proposed "heteroatomic constant potential method" (HCPM) uses minimal added parameters to handle differing electronegativities and chemical hardnesses of different elements, which we fit to density functional theory (DFT) partial charge predictions in this paper by using derivative-free optimization. To demonstrate the model, we performed molecular dynamics simulations using both HCPM and conventional constant potential method (CPM) for MXene electrodes with Li-TFSI/AN (lithium bis(trifluoromethane sulfonyl)imide/acetonitrile)-based solvent-in-salt electrolytes. Although the two methods show similar accumulated charge storage on the electrodes, the results indicated that HCPM provides a more reliable depiction of electrode atom charge distribution and charge response compared with CPM, accompanied by increased cationic attraction to the MXene surface. These results highlight the influence of elemental composition on electrode performance, and the flexibility of our HCPM opens up new avenues for studying the performance of diverse heteroatomic electrodes including other types of MXenes, two-dimensional materials, metal-organic frameworks (MOFs), and doped carbonaceous electrodes.

Cathartocytosis: How Cells Jettison Unwanted Material as They Reprogram.

Injury can cause differentiated cells to undergo massive reprogramming to become proliferative to repair tissue via a cellular program called paligenosis. Gastric digestive-enzyme-secreting chief cells use paligenosis to reprogram into progenitor-like Spasmolytic-Polypeptide Expressing Metaplasia (SPEM) cells. Stage 1 of paligenosis is to downscale mature cell architecture via a process involving lysosomes. Here, we noticed that sulfated glycoproteins (which are metaplasia and cancer markers in mice and humans) were not digested during paligenosis but excreted into the gland lumen. Various genetic and pharmacological approaches showed that endoplasmic reticulum membranes and secretory granule cargo were also excreted and that the process proceeded in parallel with, but was independent lysosomal activity. 3-dimensional light and electron-microscopy demonstrated that excretion occurred via unique, complex, multi-chambered invaginations of the apical plasma membrane. As this lysosome-independent cell cleansing process does not seem to have been priorly described, we termed it "cathartocytosis". Cathartocytosis allows a cell to rapidly eject excess material (likely in times of extreme stress such as are induced by paligenosis) without waiting for autophagic and lysosomal digestion. We speculate the ejection of sulfated glycoproteins (likely mucins) would aid in downscaling and might also help bind and flush pathogens (like H pylori which causes SPEM) away from tissue.

Super-tough and self-healable all-cellulose-based electrolyte for fast degradable quasi-solid-state supercapacitor.

Recyclable and degradable supercapacitors have promising applications for a sustainable energy storage industry. Herein, we prepare a dual-physical crosslinking (DP) carboxymethyl cellulose (CMC) hydrogel with high-toughness, healability, and electric conductivity by integrating abundant ions into the matrix. The prepared hydrogel displays a maximum compressive fracture stress of 4.42 MPa, fast healing in five seconds, and full degradation within eight days. Moreover, the fabricated supercapacitor shows high specific capacitance (309 F g-1) and volumetric capacitance (2.60 F cm-3). The supercapacitor achieves a healing efficiency of 93.9 % after five cuttings, and exhibits a cycling stability of 84.6 % capacitance retention after 1000 cycles. These merits ensure that the all-cellulose-based supercapacitor can operate in case of sudden collision and deformation, which contribute to reducing the environmental hazards from supercapacitor's preparation to its abandonment.

Wearable Triboelectric Nanogenerator with Ground-Coupled Electrode for Biomechanical Energy Harvesting and Sensing.

Harvesting biomechanical energy for electricity as well as physiological monitoring is a major development trend for wearable devices. In this article, we report a wearable triboelectric nanogenerator (TENG) with a ground-coupled electrode. It has a considerable output performance for harvesting human biomechanical energy and can also be used as a human motion sensor. The reference electrode of this device achieves a lower potential by coupling with the ground to form a coupling capacitor. Such a design can significantly improve the TENG's outputs. A maximum output voltage up to 946 V and a short-circuit current of 36.3 µA are achieved. The quantity of the charge that transfers during one step of an adult walking reaches 419.6 nC, while it is only 100.8 nC for the separate single-electrode-structured device. In addition, using the human body as a natural conductor to connect the reference electrode allows the device to drive the shoelaces with integrated LEDs. Finally, the wearable TENG is able to perform motion monitoring and sensing, such as human gait recognition, step count and movement speed calculation. These show great application prospects of the presented TENG device in wearable electronics.

Biocompatible carboxymethyl cellulose-based super-elastic hierarchical sponge via a novel templating and plasticizing method.

Herein, a facile method to fabricate hierarchical super-elastic (SE) sponge using a water-soluble cellulose derivative, carboxymethyl cellulose (CMC), is reported. The method includes ice templating and porogen leaching steps which facilitate to generate macro-sized pores as well as pore wall structures that can dissipate stress effectively. By controlling the porogen content, the specific surface area and the morphology of the sponges can be tuned. Furthermore, a plasticizing method was used before vacuum drying to reduce the deformation of the inner structure. The derived hierarchical SE CMC sponges exhibit excellent fatigue resistance, fast shape recovery, high-water absorption, biosafeness, and fast degradation. Thus, our strategy provides a novel method for the construction of SE sponges which show great potential in green elastic wound dressing, tissue engineering, and absorbent materials.

Structure-Dynamics Interrelation Governing Charge Transport in Cosolvated Acetonitrile/LiTFSI Solutions.

Concentrated ionic solutions present a potential improvement for liquid electrolytes. However, their conductivity is limited by high viscosities, which can be attenuated via cosolvation. This study employs a series of experiments and molecular dynamics simulations to investigate how different cosolvents influence the local structure and charge transport in concentrated lithium bis(trifluoromethane-sulfonyl)imide (LiTFSI)/acetonitrile solutions. Regardless of whether the cosolvent's dielectric constant is low (for toluene and dichloromethane), moderate (acetone), or high (methanol and water), they preserve the structural and dynamical features of the cosolvent-free precursor. However, the dissimilar effects of each case must be individually interpreted. Toluene and dichloromethane reduce the conductivity by narrowing the distribution of Li+-TFSI- interactions and increasing the activation energies for ionic motions. Methanol and water broaden the distributions of Li+-TFSI- interactions, replace acetonitrile in the Li+ solvation, and favor short-range Li+-Li+ interactions. Still, these cosolvents strongly interact with TFSI-, leading to conductivities lower than that predicted by the Nernst-Einstein relation. Finally, acetone preserves the ion-ion interactions from the cosolvent-free solution but forms large solvation complexes by joining acetonitrile in the Li+ solvation. We demonstrate that cosolvation affects conductivity beyond simply changing viscosity and provide fairly unexplored molecular-scale perspectives regarding structure/transport phenomena relation in concentrated ionic solutions.

Combined effects of ezetimibe and phytosterols on cholesterol metabolism: a randomized, controlled feeding study in humans.

BACKGROUND: Both ezetimibe and phytosterols inhibit cholesterol absorption. We tested the hypothesis that the combination of ezetimibe and phytosterols is more effective than ezetimibe alone in altering cholesterol metabolism. METHODS AND RESULTS: Twenty-one mildly hypercholesterolemic subjects completed a randomized, double-blind, placebo-controlled, triple-crossover study. Each subject received a phytosterol-controlled diet plus (1) ezetimibe placebo+phytosterol placebo, (2) 10 mg/d ezetimibe+phytosterol placebo, and (3) 10 mg/d ezetimibe+2.5 g phytosterols for 3 weeks each. All meals were prepared in a metabolic kitchen. Primary outcomes were intestinal cholesterol absorption, fecal cholesterol excretion, and low-density lipoprotein cholesterol levels. The combined treatment resulted in significantly lower intestinal cholesterol absorption (598 mg/d; 95% confidence interval [CI], 368 to 828) relative to control (2161 mg/d; 95% CI, 1112 to 3209) and ezetimibe alone (1054 mg/d; 95% CI, 546 to 1561; both P<0.0001). Fecal cholesterol excretion was significantly greater (P<0.0001) with combined treatment (962 mg/d; 95% CI, 757 to 1168) relative to control (505 mg/d; 95% CI, 386 to 625) and ezetimibe alone (794 mg/d; 95% CI, 615 to 973). Plasma low-density lipoprotein cholesterol values during treatment with control, ezetimibe alone, and ezetimibe+phytosterols averaged 129 mg/dL (95% CI, 116 to 142), 108 mg/dL (95% CI, 97 to 119), and 101 mg/dL (95% CI, 90 to 112; (P<0.0001 relative to control). CONCLUSION: The addition of phytosterols to ezetimibe significantly enhanced the effects of ezetimibe on whole-body cholesterol metabolism and plasma low-density lipoprotein cholesterol. The large cumulative action of combined dietary and pharmacological treatment on cholesterol metabolism emphasizes the potential importance of dietary phytosterols as adjunctive therapy for the treatment of hypercholesterolemia. CLINICAL TRIAL REGISTRATION: URL: http://www.clinicaltrials.gov. Unique identifier: NCT00863265.

Effects of nuclear factor-κB signaling pathway on periodontal ligament stem cells under lipopolysaccharide-induced inflammation.

Lipopolysaccharide (LPS) induces inflammatory stress and apoptosis. This study focused on the effect of nuclear factor kappa B (NF-κB) signaling pathway on proliferation and osteogenic differentiation of human periodontal ligament stem cells (hPDLSCs) after LPS induction and its mechanism. We first isolated hPDLSCs from human tooth root samples in vitro. Then, flow cytometry detected positive expression of cell surface antigens CD146 and STRO-1 and negative expression of CD45, suggesting the hPDLSCs were successfully isolated. LPS significantly induced increased apoptosis and diminished proliferation of hPDLSCs. The NF-κB pathway agonist phorbol 12-myristate 13-acetate (PMA) or p65 overexpression inhibited the proliferation of LPS-treated hPDLSCs and promoted apoptosis. PMA also promoted LPS-induced up-regulation of the expression of inflammatory factors TNF-α and IL-6 and down-regulation of the expression of anti-inflammatory factor IL-10. Additionally, LPS was confirmed to lead to a reduction of alkaline phosphatase (ALP) activity, calcium nodules, and expression of osteogenic markers Runt-related transcription factor 2 (Runx2) and osteopontin. This reduction could be promoted by PMA. Western blotting further indicated that PMA could promote LPS-induced decrease of expression of p65 (cytoplasm), and total cellular proteins IKKα and IKKß in hPDLSCs, while protein expression of p-IκBα (cytoplasm) and p65 (nucleus), and p-IκBα/IκBα ratio was elevated. By contrast, inhibition of the NF-κB pathway (PDTC) or small-interfering RNA targeting NF-κB/p65 (p65 siRNA) showed the opposite results. In conclusion, activation of NF-κB signaling in LPS-induced inflammatory environment can inhibit the proliferation and osteogenic differentiation of hPDLSCs. This study provides a theory foundation for the clinical treatment of periodontitis.

NMR and Theoretical Study of In-Pore Diffusivity of Ionic Liquid-Solvent Mixtures.

Despite having a lower energy density than common batteries, electric double-layer capacitors (EDLCs) offer several advantages for high-power applications, including high power density, quick charge and discharge time, and long cycle life. Room-temperature ionic liquids (RTILs) have been intensely studied as promising electrolytes for applications in ELDCs because of their wide potential window, low volatility, as well as thermal and chemical stability. The main deficiency of neat RTILs in such applications is the sluggish diffusivity, which restricts the EDLCs' power density. To alleviate the slow diffusivity, RTILs can be used in a mixture with organic solvents. In this study, we applied two-dimensional exchange nuclear magnetic resonance spectroscopy (2D EXSY NMR) and molecular dynamics (MD) simulations to investigate the diffusivity of anions of an RTIL, namely, 1-butyl-3-methyl-imidazolium bis(trifluoromethylsulfonyl)imide (BMIM+-TFSI-), dissolved in five different organic solvents, in the micropores of activated carbon. We determined that the relative concentrations of ions in solutions in the micropores were higher than those in the bulk solutions and were also solvent-dependent. The ion diffusivities in the pores were found to be almost 2 orders of magnitude slower than in the bulk solutions, with methanol showing the largest relative disparity. These results suggested that the interactions of solvents with the activated carbon are critical not only to the power density of EDLCs but also to the energy density. The comparisons of ion diffusivities between the experiments and the MD simulations suggest the need to consider also the surface functionalities of activated carbon for the simulation of ion diffusion in the micropores of activated carbon.

Room temperature preparation of cellulose nanocrystals with high yield via a new ZnCl2 solvent system.

Here, a facile method to fabricate cellulose nanocrystals (CNCs) with high yield from microcrystalline cellulose (MCC) at room temperature (RT) is achieved by using a new solvent system of zinc chloride (ZnCl2) and a little amount of hydrochloric acid (HCl). Compared with sulphuric acid hydrolysis process, about one-fifth mole of acid is used for per gram of CNCs in our protocol. CNCs with rod-like morphology are regenerated with a maximum yield of 35.2% and high crystallinity of 73.8%. Moreover, with an additional 2 h of ball-milling, the yield of CNCs could significantly increase to 66.9% at RT. The possible formation mechanism for CNCs prepared by the solvent system of ZnCl2/HCl is proposed. As the first example of isolation of CNCs with high yield at RT using ZnCl2, this work provides a facile, energy-saving, and practical strategy for the preparation of cellulose nanomaterials.

Controlling the Ion Transport Number in Solvent-in-Salt Solutions.

Solvent-in-salt (SIS) systems present promising materials for the next generation of energy storage applications. The ion dynamics is significantly different in these systems from that of ionic liquids and diluted salt solutions. In this study, we analyze the ion dynamics of two salts, Li-TFSI and Li-FSI, in highly concentrated aqueous and acetonitrile solutions. We performed high-frequency dielectric measurements covering the range of up to 50 GHz and molecular dynamics simulations. The analysis of the conductivity spectra provides the characteristic crossover time between individual charge rearrangements and the normal charge diffusion regime resulting in DC conductivity. Analysis revealed that the onset of normal charge diffusion occurs at the scale of ∼1.5-3.5 Å, comparable to the average distance between the ions. Based on the idea of momentum conservation, distinct ion correlations were estimated experimentally and computationally. The analysis revealed that cation-anion correlations can be suppressed by changing the solvent concentration in SIS systems, leading to an increase of the light ion (Li+ in our case) transport number. This discovery suggests a way for improving the light cation transport number in SIS systems by tuning the solvent concentration.

Direct Correlation of the Salt-Reduced Diffusivities of Organic Solvents with the Solvent's Mole Fraction.

Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in organic solvents (especially propylene carbonate) has demonstrated extraordinary pseudocapacitive performance as an electrolyte in the supercapacitor configuration ( Nat. Energy 2019, 4, 241-248). However, the influence of the solvated ions on the diffusivity of the solvent molecules is yet to be understood. We examine the impact of LiTFSI on the diffusivity in five organic solvents: acetonitrile (ACN), tetrahydrofuran (THF), methanol (MeOH), dimethyl sulfoxide (DMSO), and propylene carbonate (PC) using a combination of neutron scattering, conductivity measurements, and molecular dynamics simulations. The extent of the diffusivity reduction in the concentration regime of ≤1 M directly correlates with the solvent mole fraction at which the solvation shells around Li+ ions are of similar size in all the solvents, resulting in a universal ∼50% reduction in the solvent diffusivity. These results provide guidance for formulation of the new electrolytes to enhance the performance of energy storage devices.