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1.
Int J Biol Macromol ; 280(Pt 1): 135598, 2024 Sep 12.
Artigo em Inglês | MEDLINE | ID: mdl-39276878

RESUMO

This study proposed a novel extraction method for soy protein isolate, which involved solid-state fermentation of high-temperature soybean meal. The proteinases secreted by microorganisms acted on the high-temperature soybean meal, making the SPI easier to extract. The study concludes that Bacillus amyloliquefaciens subsp. plantarum CICC 10265 could be used for solid-state fermentation of soybean meal, and the fermentation effect was good, with a yield of 41.91 % for SPI. Compared to the direct extraction of SPI from high-temperature soybean meal, the yield had increased by 130.19 %. Meanwhile, we also conducted research on the losses during the SPI extraction process. Through experiments, the study identified the patterns of protease activity changes and microbial colony growth during solid-state fermentation of soybean meal by Bacillus amyloliquefaciens subsp. plantarum CICC 10265. It was concluded that extracting SPI after 8 h of fermentation is more suitable. The experimental results indicated that the total amino acid content of SPI extracted from fermented soybean meal was 2.1 % higher compared to SPI extracted from low-temperature soybean meal. The extracted SPI also met the microbial standards.

2.
ACS Appl Mater Interfaces ; 16(36): 47571-47580, 2024 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-39223875

RESUMO

To achieve large-scale hydrogen storage for growing high energy density and long-life demands in end application, the 2LiBH4-MgH2 (LMBH) reactive hydride system attracts huge interest owing to its high hydrogen capacity and thermodynamically favorable reversibility. The sluggish dehydrogenation kinetics and unsatisfactory cycle life, however, remain two challenges. Herein, a bimetallic titanium-niobium oxide with a two-dimensional nanoflake structure (2D TiNb2O7) is selected elaborately as an active precursor that in situ transforms into TiB2 and NbB2 with ultrafine size and good dispersion in the LMBH system as highly efficient catalysts, giving rise to excellent kinetic properties with long-term cycling stability. For the LMBH system added with 5 wt% 2D TiNb2O7, 9.8 wt% H2 can be released within 20 min at 400 °C, after which the system can be fully hydrogenated in less than 5 min at 350 °C and 10 MPa H2. Moreover, a dehydrogenation capacity of 9.4 wt% can be maintained after 50 cycles corresponding to a retention of 96%, being the highest reported to date. The positive roles of TiB2 and NbB2 for kinetics and recyclability are from their catalytic nucleation effects for MgB2, a main dehydrogenation phase of LMBH, thus reducing the apparent activation energy, suppressing the formation of thermostable Li2B12H12 byproducts, and inhibiting the hydride coarsening. This work develops an advanced LMBH system, bringing hope for high-capacity, fast-response, and long-life hydrogen energy storage.

3.
Luminescence ; 39(9): e4905, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39323066

RESUMO

To investigate the impact of PO4 3- anionic groups, the trivalent europium ion-doped calcium molybdate (CaMoO3-PO4:xEu3+, where x = 0.5, 1.0, 1.5, 2.0, and 2.5 mol%) phosphors were synthesized using the solid-state reaction method. The detailed study of the phosphor materials was carried out by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), optical diffuse reflectance spectroscopy (DRS), and photoluminescence (PL) spectroscopy. The XRD results indicate that the substitution of PO4 3- anion and Eu3+ dopant ion did not affect the crystal structures of the CaMoO4 phosphors. Ultraviolet-visible (UV-vis) absorption analysis revealed the change of absorption edge of both un-doped and Eu3+-doped CaMoO4-PO4 phosphors. Under the 394 nm UV-excitation, the recorded PL spectra showed an intense peak at 615 nm corresponding to the Eu3+: 5D0 → 7F2 transition. The results of the Commission Internationale de l'Eclairage (CIE) diagram reported that the color of the emissions lies in the red color zone and there is no change in the CIE coordinates of the overall emission for Eu3+-doped CaMoO4-PO4 as Eu concentration changes. Thus, these observations led to finding the best red components for white light-emitting diode applications.


Assuntos
Európio , Substâncias Luminescentes , Molibdênio , Molibdênio/química , Európio/química , Substâncias Luminescentes/química , Substâncias Luminescentes/síntese química , Luminescência , Fosfatos/química , Medições Luminescentes , Íons/química , Cálcio/química , Difração de Raios X , Espectroscopia de Infravermelho com Transformada de Fourier
4.
Curr Drug Metab ; 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39323345

RESUMO

INTRODUCTION: This study aims to develop co-amorphous Solid Dispersion (SD) system containing antimalarials Artesunate (ARS) and Amodiaquine (AMQ) to improve its oral bioavailability employing the Hot Melt Extrusion (HME) technique. Soluplus® was selected as a polymeric excipient, whereas Lutrol F127, Lutrol F68, TPGS, and PEG400 as surfactants were incorporated along with Soluplus® to enhance extrudability, improve hydrophilicity, and improve the blend viscosity during HME. Soluplus® with surfactant combination successfully stabilizes both drugs during extrusion by generating SD because of its lower glass transition temperature (Tg) and viscoelastic behavior. METHODS: Physicochemical characterizations were performed using FTIR, DSC, TGA, and XRD, which confirmed the amorphousization of drugs in the SD system. The molecular level morphology of the optimized formulation was quantified using high-resolution techniques such as Atomic-Force Microscopy (AFM), Raman spectral, and mapping analysis. The transition of the crystalline drugs into a stable amorphous form has been demonstrated by 1H-NMR and 2D-NMR studies. The in vivo pharmacokinetics study in rats showed that the SD-containing drug-Soluplus-TPGS (FDC10) formulation has 36.63-56.13 (ARS-AMQ) folds increase in the Cmax and 41.87-54.34 (ARS-AMQ) folds increase AUC(0-72) as compared to pure drugs. RESULTS: Pharmacokinetic analysis shows that a fixed-dose combination of 50:135 mg of both APIs (ARSAMQ) significantly increased oral bioavailability by elevating Cmax and AUC, in comparison to pure APIs and also better than the marketed product Coarsucam®. CONCLUSION: Therefore, the developed melt extruded co-amorphous formulation has enhanced bioavailability and has more effectiveness than the marketed product Coarsucam®

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5.
ACS Nano ; 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39324749

RESUMO

Superionic conductor-based solid-state electrolytes with preferred crystal structures hold great promise for realizing ultrafast lithium-ion (Li+) transfer, which is urgently desired for all-solid-state lithium batteries. However, the precise control of crystal growth of superionic conductors is still challenging since the crystals always spontaneously grow to disordered structures with the lowest internal energy to ensure thermodynamic stability. Herein, a coaxial nanowire with a polyvinylpyrrolidone (PVP) sheath and a Li0.33La0.557TiO3 (LLTO) precursor core (PVP/LLTO-caNW) is prepared through coaxial electrospinning, followed by sintering into LLTO nanowire with an oriented crystal structure (LLTO-caNW). We demonstrate that the one-dimensional PVP sheath as a sacrificial layer generates uniform and the strongest adsorption ability on the (110) phase among different LLTO crystal planes, which induces the crystal to preferentially grow along the c-axis (the fastest Li+ transfer direction) during the nucleation and growth processes. As a result, the prepared LLTO-caNW displays an ultrahigh bulk ionic conductivity of 3.13 × 10-3 S cm-1, exceeding most LLTO crystals and approaching the theoretical conductivity. Meanwhile, the oriented crystal growth imparts to LLTO-caNW significantly reduced grain boundary resistance, and the grain-boundary conductivity reaches up to 1.09 × 10-3 S cm-1. This endows the composite solid electrolyte with high ionic conduction performance and superior cycle stability in the assembled all-solid-state lithium battery.

6.
Nanomicro Lett ; 17(1): 21, 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39325321

RESUMO

Regulation the electronic density of solid-state electrolyte by donor-acceptor (D-A) system can achieve highly-selective Li+ transportation and conduction in solid-state Li metal batteries. This study reports a high-performance solid-state electrolyte thorough D-A-linked covalent organic frameworks (COFs) based on intramolecular charge transfer interactions. Unlike other reported COF-based solid-state electrolyte, the developed concept with D-A-linked COFs not only achieves electronic modulation to promote highly-selective Li+ migration and inhibit Li dendrite, but also offers a crucial opportunity to understand the role of electronic density in solid-state Li metal batteries. The introduced strong electronegativity F-based ligand in COF electrolyte results in highly-selective Li+ (transference number 0.83), high ionic conductivity (6.7 × 10-4 S cm-1), excellent cyclic ability (1000 h) in Li metal symmetric cell and high-capacity retention in Li/LiFePO4 cell (90.8% for 300 cycles at 5C) than substituted C- and N-based ligands. This is ascribed to outstanding D-A interaction between donor porphyrin and acceptor F atoms, which effectively expedites electron transferring from porphyrin to F-based ligand and enhances Li+ kinetics. Consequently, we anticipate that this work creates insight into the strategy for accelerating Li+ conduction in high-performance solid-state Li metal batteries through D-A system.

7.
J Mol Biol ; 436(22): 168792, 2024 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-39270971

RESUMO

The 91 kDa oligomeric ring-shaped ligand binding protein TRAP (trp RNA binding attenuation protein) regulates the expression of a series of genes involved in tryptophan (Trp) biosynthesis in bacilli. When cellular Trp levels rise, the free amino acid binds to sites buried in the interfaces between each of the 11 (or 12, depending on the species) protomers in the ring. Crystal structures of Trp-bound TRAP show the Trp ligands are sequestered from solvent by a pair of loops from adjacent protomers that bury the bound ligand via polar contacts to several threonine residues. Binding of the Trp ligands occurs cooperatively, such that successive binding events occur with higher apparent affinity but the structural basis for this cooperativity is poorly understood. We used solution methyl-TROSY NMR relaxation experiments focused on threonine and isoleucine sidechains, as well as magic angle spinning solid-state NMR 13C-13C and 15N-13C chemical shift correlation spectra on uniformly labeled samples recorded at 800 and 1200 MHz, to characterize the structure and dynamics of the protein. Methyl 13C relaxation dispersion experiments on ligand-free apo TRAP revealed concerted exchange dynamics on the µs-ms time scale, consistent with transient sampling of conformations that could allow ligand binding. Cross-correlated relaxation experiments revealed widespread disorder on fast timescales. Chemical shifts for methyl-bearing side chains in apo- and Trp-bound TRAP revealed subtle changes in the distribution of sampled sidechain rotameric states. These observations reveal a pathway and mechanism for induced conformational changes to generate homotropic Trp-Trp binding cooperativity.

8.
Adv Mater ; : e2407009, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39328019

RESUMO

Elastocaloric cooling is one of the most promising solid-state cooling approaches to address the issues of energy shortage and global warming. However, the cooling efficiency and cycle life of this technology need to be improved, and the required driving force shall be reduced. Here, a novel elastocaloric heat pump by periodic non-linear stress is developed by employing fiber twisting and separated cooling and heating media. The non-linear stress generated by fiber twisting yields a hierarchical, rigid-yet-flexible architecture and a periodic entropy spatial distribution, which result in a low mechanical hysteresis work and a high cooling efficiency (a maximum material coefficient of performance (COP) of 30.8 and a maximum Carnot efficiency of 82%). The torsional non-linear stress inhibits crack propagation and results in a highly extended cycle life (14752 cycles, more than ten times of fiber stretching). The heat pump exhibits a maximum average temperature span of 25.6 K, a maximum specific cooling power of 1850 W Kg-1, a maximum device COP of 19.5, and a maximum device power of 5.0 W, under each optimal condition.

9.
Artigo em Inglês | MEDLINE | ID: mdl-39316097

RESUMO

Enhancing iridium (Ir)-based electrocatalysts to achieve high activity and robust durability for the oxygen evolution reaction (OER) in acidic environments has been an ongoing mission in the commercialization of proton exchange membrane (PEM) electrolyzers. In this study, we present the synthesis of carbon-supported Ir nanoparticles (NPs) using a modified impregnation method followed by solid-state reduction, with Ir loadings of 20 and 40 wt % on carbon. Among the catalysts, the sample with an Ir loading of 20 wt % synthesized at 1000 °C with a heating rate of 300 °C/h demonstrated the highest mass-normalized OER performance of 1209 A gIr-1 and an OER current retention of 80% after 1000 cycles of cyclic voltammetry (CV). High-resolution STEM images confirmed the uniform dispersion of NPs, with diameters of 1.6 ± 0.4 nm across the support. XPS analysis revealed that the C-O and C═O peaks shifted slightly toward higher binding energies for the best-performing catalyst. In comparison, the metallic Ir state shifted toward lower binding energies compared to other samples. This suggests electron transfer from the carbon support to the Ir NPs, indicating a potential interaction between the catalyst and the support. This work underscores the strong potential of the solid-state method for the scalable synthesis of supported Ir catalysts.

10.
J Colloid Interface Sci ; 678(Pt C): 682-689, 2024 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-39307057

RESUMO

All-solid-state (ASS) lithium-sulfur (LiS) batteries utilizing composite polymer electrolytes (CPEs) represent a promising avenue in the domain of electric vehicles and large-scale energy storage systems, leveraging the combined benefits of polymer electrolytes (PEs) and ceramic electrolytes (CEs). However, the inherent weak interface compatibility between PEs and CEs often leads to phase separation, thereby impeding the transposition of Li+. In this study, the trimethoxy-[3-(2-methoxyethoxy)propyl]silane (TM-MES) is introduced as a chemical agent to form bonds with polyethylene oxide (PEO) and Li10GeP2S12 (LGPS), resulting in the development of a novel composite polymer electrolyte (CPETM-MES). This innovative approach mitigates phase separation between PEs and CEs while concurrently enhancing the protective capabilities of LGPS against decomposition at the interfaces of both the Li anode and sulfur cathode. Moreover, the CPETM-MES exhibits superior mechanical toughness, an expanded electrochemical window, and elevated ionic conductivity. In the symmetric cell, it demonstrates an extended operational lifespan exceeding 1800 h, and the current density can reach up to 1.05 mA/cm2. Furthermore, the initial discharge capacity of ASS LiS batteries utilizing CPETM-MES attains 1227 mAh/g and maintains a capacity of 904 mAh/g after 100 cycles. Notably, a high-energy-density of 2454 Wh/kg is achieved based on the sulfur cathode.

11.
Artigo em Inglês | MEDLINE | ID: mdl-39322220

RESUMO

All-solid-state fluoride batteries have the potential to achieve energy densities significantly higher than those of lithium-ion batteries. A common cathode material for fluoride batteries is Cu. Cu has a low polarization, but its rapid capacity degradation due to grain growth and subsequent delamination from the solid-state electrolyte are critical issues. To enhance the performance of Cu-based cathodes in all-solid-state fluoride batteries, we explore alloying of Cu with Ni to create metastable solid solution phases (CuxNi1-x with x = 0, 0.32, 0.52, 0.72, 0.89, and 1.0). Compared to Cu, Ni has a higher polarization but exhibits superior capacity retention. The Cu0.72Ni0.28 alloy demonstrates a polarization as low as Cu, but it has a significantly improved capacity retention, which is comparable to Ni. Transmission electron microscopy observations demonstrate that the thin Ni-rich region formed near the interface inhibits Cu grain growth and delamination from the LaF3 electrolyte. By incorporating an appropriate amount of Ni into Cu, Cu-Ni alloy films combine the advantages of both metals, improving the performance of fluoride batteries.

12.
Protein Sci ; 33(10): e5168, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39276003

RESUMO

The tropomyosin 1 isoform I/C C-terminal domain (Tm1-LC) fibril structure is studied jointly with cryogenic electron microscopy (cryo-EM) and solid state nuclear magnetic resonance (NMR). This study demonstrates the complementary nature of these two structural biology techniques. Chemical shift assignments from solid state NMR are used to determine the secondary structure at the level of individual amino acids, which is faithfully seen in cryo-EM reconstructions. Additionally, solid state NMR demonstrates that the region not observed in the reconstructed cryo-EM density is primarily in a highly mobile random coil conformation rather than adopting multiple rigid conformations. Overall, this study illustrates the benefit of investigations combining cryo-EM and solid state NMR to investigate protein fibril structure.


Assuntos
Microscopia Crioeletrônica , Ressonância Magnética Nuclear Biomolecular , Tropomiosina , Microscopia Crioeletrônica/métodos , Ressonância Magnética Nuclear Biomolecular/métodos , Tropomiosina/química , Tropomiosina/ultraestrutura , Modelos Moleculares , Estrutura Secundária de Proteína , Conformação Proteica
13.
Biophys Rep ; 10(4): 201-212, 2024 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-39281198

RESUMO

Sedimentation solid-state NMR is a novel method for sample preparation in solid-state NMR (ssNMR) studies. It involves the sedimentation of soluble macromolecules such as large protein complexes. By utilizing ultra-high centrifugal forces, the molecules in solution are driven into a high-concentrated hydrogel, resulting in a sample suitable for solid-state NMR. This technique has the advantage of avoiding the need for chemical treatment, thus minimizing the loss of sample biological activity. Sediment ssNMR has been successfully applied to a variety of non-crystalline protein solids, significantly expanding the scope of solid-state NMR research. In theory, using this method, any biological macromolecule in solution can be transferred into a sedimented solute appropriate for solid-state NMR analysis. However, specialized equipment and careful handling are essential for effectively collecting and loading the sedimented solids to solid-state NMR rotors. To improve efficiency, we have designed a series of loading tools to achieve the loading process from the solution to the rotor in one step. In this paper, we illustrate the sample preparation process of sediment NMR using the H1.4-NCP167 complex, which consists of linker histone H1.4 and nucleosome core particle, as an example.

15.
Animal ; 18(10): 101176, 2024 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-39299043

RESUMO

Aging reduces the nutritional value of corn grain, which may be improved by fermentation prior to use. This study investigated the effects of replacing conventional corn (CC) with aging corn (AC) and fermented aging corn (FAC) in the diets of lactating Holstein cows. Six healthy third-parity Holstein cows were used in a replicated 3 × 3 Latin square experiment with 21-day periods. Cows were fed twice and milked twice daily. The cows were randomly divided into three treatment groups: (1) CC diet: a diet with 23.6% starch in diet DM containing 24.0% conventional corn; (2) AC diet: a diet with 23.5% starch in diet DM containing 24.0% aging corn replacing conventional corn; and (3) FAC diet: a diet with 23.2% starch in diet DM containing 24.6% fermented aging corn replacing conventional corn. The diets were formulated to be isonitrogenous and contained identical roughage. The FAC treatment increased the starch digestibility compared with AC. Feeding FAC increased the concentrations of total volatile fatty acid compared with CC and AC and decreased the molar proportion of acetate compared with AC. At the family level, the relative abundance of Prevotellaceae was higher on FAC than CC. The relative abundance of Succinivibrionaceae was lower on FAC than on CC and AC. Besides, at the genera level, the relative abundance of Succinivibrionaceae_UCG_002 in the rumen was higher on AC than CC and FAC. The relative abundance of Prevotella and Ruminococcus was higher on FAC than CC and AC. The relative abundance of Succinivibrionaceae_UCG_001 was lower on FAC than CC. The Simpson index was lower on FAC than CC and AC. The FAC treatment increased the milk yield (34.0, 33.7, and 35.2 kg/d for CC, AC, and FAC group, respectively) and protein yield, and thus, energy-corrected milk production was increased, and at the same time, decreased the somatic cell score compared with CC and AC. The AC treatment increased the malondialdehyde concentration in plasma compared with CC and FAC. The concentrations in plasma of triglyceride and malondialdehyde were lower on FAC than AC. The immunoglobulin G concentration in plasma was higher on FAC than CC and AC. Overall, feeding AC resulted in decreased plasma antioxidant capacity compared with CC, whereas feeding FAC altered the relative abundance of bacteria in the rumen and improved starch digestibility, ruminal bacterial diversity, lactation performance, plasma antioxidant capacity and immune competence compared with AC in dairy cows.

16.
ACS Appl Bio Mater ; 7(9): 5795-5809, 2024 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-39279416

RESUMO

Narrow band red-emitting phosphors based on organo-Eu(III) complexes prove their energetic features with surprising performance in smart red/white LEDs, sensing, and biological fields. In this report, a series of unique Eu(III) complexes have been synthesized with coumarin integrated with a class of phenanthroline(Phen)/thiabendazole(TBZ) based ancillary ligands and dibenzoyl methane (DBM)/2-theonyl trifluoroacetone (TTA) as an anionic ligand. The computational study reveals that the TBZ/Phen-based neutral ligands are superior energy harvesters to those other reported analogue neutral ligands. All the Eu-complexes demonstrated outstanding red emission due to electric dipole (ED) transition (5D0 → 7F2) in solid, solution, and thin film with high quantum yield (QY). Theoretical analysis (TD-DFT) and experimental findings describe that the energy transfer (ET) from the ligand's triplet level to the Eu(III) ion is completely occurring. The Eu(III) complexes can potentially be used to fabricate intense hybrid white and red LEDs. All of the fabricated red LEDs revealed high luminous efficiency of radiation (LER) values. The fabricated blue LED based hybrid white LEDs displayed remarkable performance with a low correlated color temperature (5634 K), high color rendering index 88%, and CIE values (x = 0.33; y = 0.342) for 3Eu. By interaction with acid-base vapors, Eu-complexes displayed effectively alterable on-off-on luminescence. Further, cellular imaging shows that Eu-complexes can be a potential biomarker for cancer cell lines.


Assuntos
Cumarínicos , Európio , Teste de Materiais , Fenantrolinas , Európio/química , Cumarínicos/química , Humanos , Fenantrolinas/química , Estrutura Molecular , Materiais Biocompatíveis/química , Materiais Biocompatíveis/síntese química , Tamanho da Partícula , Imagem Óptica , Complexos de Coordenação/química , Complexos de Coordenação/síntese química , Medições Luminescentes , Substâncias Luminescentes/química , Substâncias Luminescentes/síntese química
17.
Small Methods ; : e2400910, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39319485

RESUMO

Garnet-type solid-state lithium batteries (SSLBs) possess excellent potential owing to their safety and high energy density. However, fundamental barriers are deficient cycling stability and poor rate capability. The main concern lies in generating voids at the Li|garnet interface during Li stripping, stemming from the sluggish diffusion of Li atoms inside the bulk Li metal. Herein, a composite anode (AN@Li) containing Li-Al alloy, Li3N, and LiNO2 is designed by introducing aluminum nitrate into molten Li. The lower interfacial formation energies exhibited by Li-Al alloy, Li3N, and LiNO2 with garnet solid-state electrolyte (SSE) enhance the wettability of AN@Li toward SSE. Meanwhile, it affords efficient conductive pathways that facilitate Li+ diffusion in the bulk anode (not just on the surface). Impressively, the resulting symmetric cell with AN@Li electrodes achieves high critical current density (1.95 mA cm-2) and long cycle life (6000 h at 0.3 mA cm-2). The SSLB coupled with LiFePO4 cathode and AN@Li anode enables stable cycling for 200 cycles at a high rate of 1 C with a retention of 96% and exhibiting outstanding rate capability (145.9 mAh g-1 at 2 C). This work provides practical insights for producing high-performance lithium metal anode for advanced garnet-type SSLBs.

18.
ACS Appl Mater Interfaces ; 16(38): 51469-51479, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39263963

RESUMO

As an important component of lithium-ion batteries, all-solid-state electrolytes should possess high ionic conductivity, excellent flexibility, and relatively high mechanical strength. All-solid-state polymer electrolytes (ASSPEs) based on polymers seem to be able to meet these requirements. However, pure ASSPEs have relatively low ionic conductivity, and the addition of inorganic fillers such as lithium salts will reduce their flexibility and mechanical strength. To address the above issues, in this paper, the solvent-free method was used to prepare a poly(vinylidenefluoride-co-hexafluoropropylene)/lithium bis(trifluoromethanesulfonyl) imide/poly(ethylene oxide) all-solid-state polymer electrolyte, which was then subjected to 4 × 4 magnification synchronous bidirectional stretching. Subsequently, it was multilayered with PEO-based composite polymer electrolytes to obtain multilayered composite polymer electrolytes (MCPEs). Bidirectional stretching provides superior in-plane and out-of-plane mechanical properties to MCPEs by inducing molecular chain orientation, which suppresses the growth of lithium dendrites. Concurrently, it facilitates the formation of the ß-crystal form of PVDF-HFP, thereby weakening the ion solvation effect and reducing the lithium-ion migration energy barrier. Multilayered compounding improves the interfacial contact between MCPEs and electrodes, thereby reducing the interfacial impedance. Experiments have demonstrated that the MCPEs prepared in this paper exhibit high ionic conductivity at room temperature (1.83 × 10-4 S cm-1), low interfacial resistance (547 Ω cm-2), excellent mechanical properties (26 MPa), and excellent cycling rate performance (a capacity retention rate of 90% after 110 cycles at 0.1 C), which can meet the performance requirements of lithium-ion batteries for ASSPEs.

19.
ACS Appl Mater Interfaces ; 16(38): 50736-50746, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39268633

RESUMO

The inevitable shift toward renewable energy and electrification necessitates earth-abundant sodium reserves for next-generation Na-based energy storage technologies. By coupling the benefits of solid electrolytes over traditional nonaqueous electrolytes due to their safety hazards, solid-state sodium-ion batteries hold huge prospects in the future. This work presents a comprehensively developed solid-state sodium-ion symmetric full cell operating at room temperature enabled through a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based polymer electrolyte and modified NASICON-structured positive and negative electrodes. Among the investigated polymer electrolytes, PVDF-HFP-NaTFSI was found to outperform other counterparts by achieving a higher ionic conductivity and delivered an appreciable electrochemical stability window. By further delving into the properties of PVDF-HFP-NaTFSI, it was found to possess the least crystallinity, minimal porous structure, lowest melting point, and fusion enthalpy, indicating better ion transport than other investigated polymer electrolytes. The as-assembled solid-state battery revealed a storage capacity of 74 mAh g-1 at 0.1 C with a specific energy density of 130 Wh kgcathode_active_material-1 and demonstrated an impressive capacity retention of 84% of the initial capacity after 200 cycles. The structure and morphology retention of the cycled electrode and electrolyte through postmortem analysis bolster the electrochemo-mechanical stability of the developed solid cell. The findings reported here on polymer electrolytes persuade expedient solutions for developing ambient temperature solid-state sodium-ion batteries with promising electrochemical performance for commercialization in the near future.

20.
ACS Appl Mater Interfaces ; 16(38): 50671-50678, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39268792

RESUMO

Sustainable batteries are key for powering electronic devices of the future, with aqueous zinc-ion batteries (AZIBs) standing out for their use of abundant, readily available elements, and safer production processes. Among the various electrode materials studied for AZIBs, the Chevrel Phase, Mo6S8 has shown promise due to its open framework, but issues with zinc ion trapping have limited its practical application. In this work, we employed computational methods to investigate the insertion-deinsertion mechanism in a series of isostructural Mo6S8-xSex (x = 0-8) solid solutions as materials that could balance the gravimetric capacity and reversible cycling for AZIBs. Density functional theory (DFT) calculations revealed that increasing the Se content would reduce the binding energy of Zn within the structures, enabling Zn deinsertion compared to the Mo6S8 structure. Experiments confirmed the formation of Mo6S8-xSex (x = 0-8) solid solutions, and electrochemical testing showed improved reversibility of Zn insertion/deinsertion as the amount of Se increased, consistent with the computational predictions. Furthermore, combined in operando X-ray diffraction and electrochemical studies revealed a continuous, gradual Zn-insertion process into Mo6S4Se4, in stark contrast to the abrupt phase changes observed upon Zn insertion in Mo6S8 and Mo6Se8. DFT calculations attributed the stabilization of Zn0.5Mo6S4Se4 as a prime reason for preventing phase separation, making Se-substituted compounds promising materials for high-performance AZIBs. Overall, this interdisciplinary approach, integrating computational modeling, materials synthesis, and advanced characterization techniques, offers a pathway for fine-tuning anion chemistry that can help create high-performance electrode materials for sustainable energy storage technologies.

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