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All-solid-state lithium batteries have attracted widespread attention for next-generation energy storage, potentially providing enhanced safety and cycling stability. The performance of such batteries relies on solid electrolyte materials; hence many structures/phases are being investigated with increasing compositional complexity. Among the various solid electrolytes, lithium halides show promising ionic conductivity and cathode compatibility, however, there are no effective guidelines when moving toward complex compositions that go beyond ab-initio modeling. Here, we show that ionic potential, the ratio of charge number and ion radius, can effectively capture the key interactions within halide materials, making it possible to guide the design of the representative crystal structures. This is demonstrated by the preparation of a family of complex layered halides that combine an enhanced conductivity with a favorable isometric morphology, induced by the high configurational entropy. This work provides insights into the characteristics of complex halide phases and presents a methodology for designing solid materials.
Ions have a profound effect on the geometrical structure of liquid water and an aqueous environment is known to change the electronic structure of ions. Here we combine photoelectron spectroscopy measurements from liquid microjets with molecular dynamical and quantum chemical calculations to address the reverse question, to what extent do ions affect the electronic structure of liquid water? We study aqueous solutions of sodium iodide (NaI) over a wide concentration range, from nearly pure water to 8 M solutions, recording spectra in the 5 to 60 eV binding energy range to include all water valence and the solute Na+ 2p, I- 4d, and I- 5p orbital ionization peaks. We observe that the electron binding energies of the solute ions change only slightly as a function of electrolyte concentration, less than 150 ± 60 meV over an ∼8 M range. Furthermore, the photoelectron spectrum of liquid water is surprisingly mildly affected as we transform the sample from a dilute aqueous salt solution to a viscous, crystalline-like phase. The most noticeable spectral changes are a negative binding energy shift of the water 1b2 ionizing transition (up to -370 ± 60 meV) and a narrowing of the flat-top shape water 3a1 ionization feature (up to 450 ± 90 meV). A novel computationally efficient technique is introduced to calculate liquid-state photoemission spectra using small clusters from molecular dynamics (MD) simulations embedded in dielectric continuum. This theoretical treatment captured the characteristic positions and structures of the aqueous photoemission peaks, reproducing the experimentally observed narrowing of the water 3a1 feature and weak sensitivity of the water binding energies to electrolyte concentration. The calculations allowed us to attribute the small binding energy shifts to ion-induced disruptions of intermolecular electronic interactions. Furthermore, they demonstrate the importance of considering concentration-dependent screening lengths for a correct description of the electronic structure of solvated systems. Accounting for electronic screening, the calculations highlight the minimal effect of electrolyte concentration on the 1b1 binding energy reference, in accord with the experiments. This leads us to a key finding that the isolated, lowest-binding-energy, 1b1, photoemission feature of liquid water is a robust energetic reference for aqueous liquid microjet photoemission studies.
High-entropy alloys/compounds have large configurational entropy by introducing multiple components, showing improved functional properties that exceed those of conventional materials. However, how increasing entropy impacts the thermodynamic/kinetic properties in liquids that are ambiguous. Here we show this strategy in liquid electrolytes for rechargeable lithium batteries, demonstrating the substantial impact of raising the entropy of electrolytes by introducing multiple salts. Unlike all liquid electrolytes so far reported, the participation of several anionic groups in this electrolyte induces a larger diversity in solvation structures, unexpectedly decreasing solvation strengths between lithium ions and solvents/anions, facilitating lithium-ion diffusivity and the formation of stable interphase passivation layers. In comparison to the single-salt electrolytes, a low-concentration dimethyl ether electrolyte with four salts shows an enhanced cycling stability and rate capability. These findings, rationalized by the fundamental relationship between entropy-dominated solvation structures and ion transport, bring forward high-entropy electrolytes as a composition-rich and unexplored space for lithium batteries and beyond.
Eight new polymerizable ammonium-TFSI ionic liquids were synthesized and characterized with respect to an application in energy storage devices. The ionic liquids feature methacrylate or acrylate termination as polymerizable groups. The preparation was optimized to obtain the precursors and ionic liquids in high yield. All products were characterized by NMR and IR spectroscopy. Phase transition temperatures were obtained by DSC analysis. Density, viscosity and ionic conductivity of the ionic liquids were compared and discussed. The results reveal that the length of attached alkyl groups as well as the methyl group at the polymerizable function have significant influences on the ionic liquids physicochemical properties. Ionic conductivity values vary between 0.264 mS cm-1 for [C₂NA,22]TFSI and 0.080 mS cm-1 for [C₈NMA,22]TFSI at 25 °C. Viscosity values are within a range of 0.762 Pa s for [C₂NA,22]TFSI and 1.522 Pa s for [C₆NMA,22]TFSI at 25 °C.
A deep eutectic solvent (DES) is an ionic liquid-analog electrolyte, newly emerging due to its low cost, easy preparation, and tunable properties. Herein, a zinc-bromine battery (ZBB) with a Zn-halide-based DES electrolyte prepared by mixing ZnBr2 , ZnCl2 , and a bromine-capturing agent is reported. The water-free DES electrolyte allows a closed-cell configuration for the ZBB owing to the prevention of Br2 evaporation and H2 evolution. It is found that the Cl- anion changes the structure of the zinc-halide complex anions and demonstrated that it improves the ion mobility and electrode reaction kinetics. The DES electrolyte with the optimized ZnCl2 composition shows much higher rate capability and a cycle life 90 times longer than that of a ZnCl2 -free DES electrolyte. A pouch-type flexible ZBB battery based on the DES electrolyte exhibits swelling-free operation for more than 120 cycles and stable operation under a folding test, suggesting its potential in consumer applications such as wearable electronics.
Ceramic/polymer composite solid electrolytes integrate the high ionic conductivity of in ceramics and the flexibility of organic polymers. In practice, ceramic/polymer composite solid electrolytes are generally made into thin films rather than sintered into bulk due to processing temperature limitations. In this work, Li6.4La3Zr1.4Ta0.6O12 (LLZTO)/polyethylene-oxide (PEO) electrolyte containing bis(trifluoromethanesulfonyl)imide (LiTFSI) as the lithium salt was successfully fabricated into bulk pellets via the cold sintering process (CSP). Using CSP, above 80% dense composite electrolyte pellets were obtained, and a high Li-ion conductivity of 2.4 × 10-4 S cm-1 was achieved at room temperature. This work focuses on the conductivity contributions and microstructural development within the CSP process of composite solid electrolytes. Cold sintering provides an approach for bridging the gap in processing temperatures of ceramics and polymers, thereby enabling high-performance composites for electrochemical systems.
Electrolytes and Lipids have always played significant roles, and changes in their concentrations gives good indications of disease progression in a number of non-communicable diseases. Diabetes mellitus is the most common metabolic disorder in the community. Diabetics may suffer from electrolyte disorders due to complications of diabetes mellitus and the medication they receive. Serum glucose, electrolytes (Na⁺, K⁺, Cl- and Ca++), and lipid profiles (total cholesterol, triglyceride, and HDL-c) were determined in 100 diabetics and in non-diabetic subjects. All the diabetic patients had a significant (p < 0.001) increase in glucose, total cholesterol, triglyceride, chloride and calcium levels. There was significant (p < 0.001) decrease in the serum levels of Na⁺ and K⁺ in all diabetics. It was concluded that differences in lipids and electrolytes found in diabetics may have great potential as a diagnostic tool in clinical practice and have a significant effect upon the risk of contracting many diseases.
In recent years, the synthesis of polymer electrolyte systems derived from biopolymers for the development of sustainable green electrochemical devices has attracted great attention. Here electrolytes based on the red seaweeds-derived polysaccharide κ-carrageenan (κ-Cg) doped with neodymium triflate (NdTrif₃) and glycerol (Gly) were obtained by means of a simple, clean, fast, and low-cost procedure. The aim was to produce near-infrared (NIR)-emitting materials with improved thermal and mechanical properties, and enhanced ionic conductivity. Cg has a particular interest, due to the fact that it is a renewable, cost-effective natural polymer and has the ability of gelling in the presence of certain alkali- and alkaline-earth metal cations, being good candidates as host matrices for accommodating guest cations. The as-synthesised κ-Cg-based membranes are semi-crystalline, reveal essentially a homogeneous texture, and exhibit ionic conductivity values 1⁻2 orders of magnitude higher than those of the κ-Cg matrix. A maximum ionic conductivity was achieved for 50 wt.% Gly/κ-Cg and 20 wt.% NdTrif₃/κ-Cg (1.03 × 10-4, 3.03 × 10-4, and 1.69 × 10-4 S cm-1 at 30, 60, and 97 °C, respectively). The NdTrif-based κ-Cg membranes are multi-wavelength emitters from the ultraviolet (UV)/visible to the NIR regions, due to the κ-Cg intrinsic emission and to Nd3+, ⁴F3/2→⁴I11/2-9/2.
The interactions between ions and lipid monolayers have captivated the attention of biologists and chemists alike for almost a century. In the absence of experimentally accessible concentration profiles, the electrolyte adsorption remains the most informative quantitative characteristic of the ion-lipid interactions. However, there is no established procedure to obtain the electrolyte adsorption on spread lipid monolayers. As a result, in the literature, the ion-lipid monolayer interactions are discussed qualitatively, based on the electrolyte effect on more easily accessible variables, e.g., surface tension. In this letter, we demonstrate how the electrolyte adsorption on lipid monolayers can be obtained experimentally. The procedure requires combining surface pressure versus molecular area compression isotherms with spreading pressure data. For the first time, we report an adsorption isotherm of NaCl on a lipid monolayer as a function of the density of the monolayer. The leading interactions seem to be the osmotic effect from the lipid head groups in the surface layer and ion-lipid association.
Pyridinium electrolytes are promising candidates for flow-battery-based energy storage1-4. However, the mechanisms underlying both their charge-discharge processes and overall cycling stability remain poorly understood. Here we probe the redox behaviour of pyridinium electrolytes under representative flow battery conditions, offering insights into air tolerance of batteries containing these electrolytes while providing a universal physico-chemical descriptor of their reversibility. Leveraging a synthetic library of extended bispyridinium compounds, we track their performance over a wide range of potentials and identify the singlet-triplet free energy gap as a descriptor that successfully predicts the onset of previously unidentified capacity fade mechanisms. Using coupled operando nuclear magnetic resonance and electron paramagnetic resonance spectroscopies5,6, we explain the redox behaviour of these electrolytes and determine the presence of two distinct regimes (narrow and wide energy gaps) of electrochemical performance. In both regimes, we tie capacity fade to the formation of free radical species, and further show that π-dimerization plays a decisive role in suppressing reactivity between these radicals and trace impurities such as dissolved oxygen. Our findings stand in direct contrast to prevailing views surrounding the role of π-dimers in redox flow batteries1,4,7-11 and enable us to efficiently mitigate capacity fade from oxygen even on prolonged (days) exposure to air. These insights pave the way to new electrolyte systems, in which reactivity of reduced species is controlled by their propensity for intra- and intermolecular pairing of free radicals, enabling operation in air.
Polymer electrolytes are attractive candidates to boost the application of rechargeable lithium metal batteries. Single-ion conducting polymers may reduce polarization and lithium dendrite growth, though these materials could be mechanically overly rigid, thus requiring ion mobilizers such as organic solvents to foster transport of Li ions. An inhomogeneous mobilizer distribution and occurrence of preferential Li transport pathways eventually yield favored spots for Li plating, thereby imposing additional mechanical stress and even premature cell short circuits. In this work, we explored ceramic-in-polymer hybrid electrolytes consisting of polymer blends of single-ion conducting polymer and PVdF-HFP, including EC/PC as swelling agents and silane-functionalized LATP particles. The hybrid electrolyte features an oxide-rich layer that notably stabilizes the interphase toward Li metal, enabling single-side lithium deposition for over 700 h at a current density of 0.1 mA cm-2. The incorporated oxide particles significantly reduce the natural solvent uptake from 140 to 38 wt % despite maintaining reasonably high ionic conductivities. Its electrochemical performance was evaluated in LiNi0.6Co0.2Mn0.2O2 (NMC622)||Li metal cells, exhibiting impressive capacity retention over 300 cycles. Notably, very thin LiNbO3 coating of the cathode material further boosts the cycling stability, resulting in an overall capacity retention of 78% over more than 600 cycles, clearly highlighting the potential of hybrid electrolyte concepts.
Divalent-cation-based batteries are being considered as potential high energy density storage devices. The optimization of electrolytes for these technologies is, however, still largely lacking. Recent demonstration of the feasibility of Ca and Mg plating and stripping in the presence of a passivation layer or an artificial interphase has paved the way for more diverse electrolyte formulations. Here, we exhaustively evaluate several Ca-based electrolytes with different salts, solvents, and concentrations, via measuring physicochemical properties and using vibrational spectroscopy. Some comparisons with Mg- and Li-based electrolytes are made to highlight the unique properties of the Ca2+ cation. The Ca-salt solubility is found to be a major issue, calling for development of new highly dissociative salts. Nonetheless, reasonable salt solubility and dissociation are achieved using bis(trifluoromethanesulfonyl)imide (TFSI), BF4, and triflate anion based electrolytes and high-permittivity solvents, such as ethylene carbonate (EC), propylene carbonate (PC), γ-butyrolactone (gBL), and N,N-dimethylformamide (DMF). The local Ca2+ coordination is concentration-dependent and rather complex, possibly involving bidentate coordination and participation of the nitrogen atom of DMF. The ionicity and the degree of ion-pair formation are both investigated and found to be strongly dependent on the nature of the cation, solvent donicity, and salt concentration. The large ion-ion interaction energies of the contact ion pairs, confirmed by density functional theory (DFT) calculations, are expected to play a major role in the interfacial processes, and thus, we here provide electrolyte design strategies to engineer the cation solvation and possibly improve the power performance of divalent battery systems.
Acetonitrile has emerged as a solvent candidate for novel electrolyte formulations in metal-ion batteries and supercapacitors. It features a bright local C≡N stretch vibrational mode whose infrared (IR) signature is sensitive to battery-relevant cations (Li+, Mg2+, Zn2+, Ca2+) both in pure form and in the presence of water admixture across a full possible range of concentrations from the dilute to the superconcentrated regime. Stationary and time-resolved IR spectroscopy thus emerges as a natural tool to study site-specific intermolecular interactions from the solvent perspective without introducing an extrinsic probe that perturbs solution morphology and may not represent the intrinsic dynamics in these electrolytes. The metal-coordinated acetonitrile, water-separated metal-acetonitrile pair, and free solvent each have a distinct vibrational signature that allows their unambiguous differentiation. The IR band frequency of the metal-coordinated acetonitrile depends on the ion charge density. To study the ion transport dynamics, it is necessary to differentiate energy-transfer processes from structural interconversions in these electrolytes. Isotope labeling the solvent is a necessary prerequisite to separate these processes. We discuss the design principles and choice of the CD313CN label and characterize its vibrational spectroscopy in these electrolytes. The Fermi resonance between 13C≡N and C-D stretches complicates the spectral response but does not prevent its effective utilization. Time-resolved two-dimensional (2D) IR spectroscopy can be performed on a mixture of acetonitrile isotopologues and much can be learned about the structural dynamics of various species in these formulations.
Codonopsis Radix is a traditional Chinese medicine best known for its effects in treating digestive, cardiovascular, immunological and hematopoitic diseases. It also appears in the traditional Chinese medical prescriptions against ascites. However, the physiological effect and molecular mechanism of Codonopsis Radix in water and electrolytes homeostasis have not been well studied. We found that Codonopsis Radix decoction increased water intake and the urine volume, but decreased food intake in mice. The treatment significantly reduced angiotensin II receptor (AT1R) transcription and serum aldosterone level in animals, suggested perturbed function of renin-angiotensin system. RNAseq analysis of Codonopsis Radix treated NCI-H295R cells detected suppressed AT1R, SP1, and TEF transcription as well. Thus, Codonopsis Radix may regulate water and electrolytes homeostasis by affecting AT1R expression and aldosterone biosynthesis, possibly through downregulating SP1 and TEF transcription.
Electrochemical cells based on alkali metal anodes are receiving intensive scientific interest as potentially transformative technology platforms for electrical energy storage. Chemical, morphological, mechanical and hydrodynamic instabilities at the metal anode produce uneven metal electrodeposition and poor anode reversibility, which, are among the many known challenges that limit progress. Here, we report that solid-state electrolytes based on crosslinked polymer networks can address all of these challenges in cells based on lithium metal anodes. By means of transport and electrochemical analyses, we show that manipulating thermodynamic interactions between polymer segments covalently anchored in the network and "free" segments belonging to an oligomeric electrolyte hosted in the network pores, one can facilely create hybrid electrolytes that simultaneously exhibit liquid-like barriers to ion transport and solid-like resistance to morphological and hydrodynamic instability.
The beverage hydration index (BHI) facilitates a comparison of relative hydration properties of beverages using water as the standard. The additive effects of electrolytes, carbohydrate, and protein on rehydration were assessed using BHI. Nineteen healthy young adults completed four test sessions in randomized order: deionized water (W), electrolytes only (E), carbohydrate-electrolytes (C + E), and 2 g/L dipeptide (alanyl-glutamine)-electrolytes (AG + E). One liter of beverage was consumed, after which urine and body mass were obtained every 60 min through 240 min. Compared to W, BHI was higher (p = 0.007) for C + E (1.15 ± 0.17) after 120 min and for AG + E (p = 0.021) at 240 min (1.15 ± 0.20). BHI did not differ (p > 0.05) among E, C + E, or AG + E; however, E contributed the greatest absolute net effect (>12%) on BHI relative to W. Net fluid balance was lower for W (p = 0.048) compared to C + E and AG + E after 120 min. AG + E and E elicited higher (p < 0.001) overall urine osmolality vs. W. W also elicited greater reports of stomach bloating (p = 0.02) compared to AG + E and C + E. The addition of electrolytes alone (in the range of sports drinks) did not consistently improve BHI versus water; however, the combination with carbohydrate or dipeptides increased fluid retention, although this occurred earlier for the sports drink than the dipeptide beverage. Electrolyte content appears to make the largest contribution in hydration properties of beverages for young adults when consumed at rest.
Either as salts or room temperature ionic liquids, fluorinated anion-based electrolytes have been a common choice for ionic electroactive polymer actuators, both linear and bending. In the present work, propylene carbonate solutions of four electrolytes of the three hugely popular anions-triflouromethanesulfonate, bis(trifluoromethane)sulfonimide, and hexafluorophosphate were compared and evaluated in polypyrrole linear actuators. The actuation direction, the characteristics-performance relations influence the behavior of the actuators. Isotonic Electro-chemo-mechanical deformation (ECMD) measurements were performed to study the response of the PPy/DBS samples. The highest strain for pristine PPy/DBS linear actuators was found in range of 21% for LiTFSI, while TBAPF6 had the least cation involvement, suggesting the potential for application in durable and controllable actuators. Interesting cation effects on the actuation of the same anions (CF3SO3-) were also observed.
Electrochemical capacitors operating in an aqueous electrolyte solution have become ever-more popular in recent years, mainly because they are cheap and ecofriendly. Additionally, aqueous electrolytes have a higher ionic conductivity than organic electrolytes and ionic liquids. These materials can exist in the form of a liquid or a solid (hydrogel). The latter form is a very promising alternative to liquid electrolytes because it is solid, which prevents electrolyte leakage. In our work, hydrogel polymer electrolytes (HPEs) were obtained via photopolymerization of a mixture of acrylic oligomer Exothane 108 with methacrylic acid (MAA) in ethanol, which was later replaced by electrolytes (1 M Na2SO4). Through the conducted research, the effects of the monomers ratio and the organic solvent concentration (ethanol) on the mechanical properties (tensile test), electrolyte sorption, and ionic conductivity were examined. Finally, hydrogel polymer electrolytes with high ionic conductivity (σ = 26.5 mS∙cm-1) and sufficient mechanical stability (σmax = 0.25 MPa, εmax = 20%) were tested using an AC/AC electrochemical double layer capacitor (EDLC). The electrochemical properties of the devices were investigated via cyclic voltammetry, galvanostatic charge/discharge, and impedance spectroscopy. The obtained results show the application potential of the obtained HPE in EDLC.
In the current study, flexible films of polyvinyl alcohol (PVA): chitosan (CS) solid polymer blend electrolytes (PBEs) with high ion transport property close enough to gel based electrolytes were prepared with the aid of casting methodology. Glycerol (GL) as a plasticizer and sodium bromide (NaBr) as an ionic source provider are added to PBEs. The flexible films have been examined for their structural and electrical properties. The GL content changed the brittle and solid behavior of the films to a soft manner. X-ray diffraction (XRD) and Fourier transform infrared (FTIR) methods were used to examine the structural behavior of the electrolyte films. X-ray diffraction investigation revealed that the crystalline character of PVA:CS:NaBr declined with increasing GL concentration. The FTIR investigation hypothesized the interaction between polymer mix salt systems and added plasticizer. Infrared (FTIR) band shifts and fluctuations in intensity have been found. The ion transport characteristics such as mobility, carrier density, and diffusion were successfully calculated using the experimental impedance data that had been fitted with EEC components and dielectric parameters. CS:PVA at ambient temperature has the highest ionic conductivity of 3.8 × 10 S/cm for 35 wt.% of NaBr loaded with 55 wt.% of GL. The high ionic conductivity and improved transport properties revealed the suitableness of the films for energy storage device applications. The dielectric constant and dielectric loss were higher at lower frequencies. The relaxation nature of the samples was investigated using loss tangent and electric modulus plots. The peak detected in the spectra of tanδ and M" plots and the distribution of data points are asymmetric besides the peak positions. The movements of ions are not free from the polymer chain dynamics due to viscoelastic relaxation being dominant. The distorted arcs in the Argand plot have confirmed the viscoelastic relaxation in all the prepared films.
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