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1.
Small ; : e2405004, 2024 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-39370658

RESUMO

The broad applications of rechargeable batteries urge people to develop alternative energy storage devices with sustainable resources, high capacity, long cycling life, and wide-temperature operability. Aqueous proton batteries are considered as a state-of-the-art energy storage system due to their intrinsic safety and low cost. However, aqueous electrolytes have a low boiling point and narrow electrochemical stability window, limiting their applications in wide-temperature and high-energy batteries. Herein, a hybrid organic ionic liquid electrolyte with organic alkali 1-methyl-1,2,4-triazole (MTA) protonated by organic acid bis(trifluoromethysulfonyl)imide (HTFSI) as proton carriers and tetramethylene sulfone (TMS) as the solvent, noted as HTFSI-MTA-TMS, exhibited the stable electrochemical windows exceeding 5 V at -20 °C and 3.5 V at 80 °C. Benefiting from this electrolyte, the assembled MnO2-S//MoO3 button proton full battery can display an operation voltage up to 1.8 V, energy density of 44.8 Wh kg-1, and good cycling stability at room temperature when bis(trifluoromethanesulfonyl)imide manganese (II) salt (Mn(TFSI)2) is introduced into the electrolyte, and run well in a wide-temperature range (-20 °C-60 °C). The work reveals the potential of organic acid-alkali coregulated electrolytes to meet the need of energy storage in a wide-temperature range and will advance the development of high-energy proton batteries.

2.
Angew Chem Int Ed Engl ; : e202414728, 2024 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-39301835

RESUMO

Aqueous Zn-ion batteries (ZIBs) have attracted attention for grid applications due to their cost-effectiveness and high security. However, their lifespan decreases at high temperatures due to declining interfacial stability and increased side reactions. To address these challenges, a ternary deep eutectic solvent-based flexible electrolyte, comprised of ZnClO4·6H2O, butanedinitrile (BD), and LiCl in an amphoteric polymer matrix, was developed to enable wide-temperature ZIBs working from -20 °C to 70 °C. The interactions among BD, Li+, and zinc hydrate alongside the amphoteric groups on the polyelectrolyte matrix could effectively suppress the interfacial side reactions and Zn dendrites formation. Consequently, the symmetric Zn cell demonstrates exceptional stability across a wide-temperature range, with the ability to survive up to 2780 hours (1 mA·cm-2) at 50 °C. Furthermore, the flexible Zn||PANI battery can operate stably over 1000 cycles at 50 °C, boasting an initial specific capacity of 124.8 mAh·g-1 and capacity retention rate of 87.9% (3 A·g-1). This work presents an effective strategy for designing high-stability energy storage devices with excellent security features that can function reliably across diverse temperature conditions.

3.
J Colloid Interface Sci ; 678(Pt B): 388-399, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-39255596

RESUMO

The traditional preparation of nanocomposite proton exchange membranes (PEM) is hindered by poor organic-inorganic interface compatibility, insufficient proton-conducting sites, easy aggregation of nanoparticles, and difficulty in leveraging nanoscale advantages. In this study, a novel method involving electrochemical anodic oxidation exfoliation was employed to prepare melamine-coated graphene oxide (Me@GO), which was subsequently subjected to in-situ polymerization with poly(2,5-benzimidazole) (ABPBI) to prepare a Me@GO/ABPBI composite proton exchange membrane. Benefiting from the strong hydrogen bonding and large π stacking interactions, melamine (Me) tightly bound to graphene oxide (GO), effectively preventing the secondary aggregation of GO after exfoliation. Moreover, the abundant alkaline functional groups of melamine enhanced the enhancement of phosphoric acid (PA) retention in the Me@GO/ABPBI membranes, thereby increasing the number of proton-conducting sites. The experimental results indicated that the introduction of Me@GO enhanced membrane properties. For Me@GO at a concentration of 1 wt%, the tensile strength of the 1Me@GO/ABPBI composite membrane reached 207 MPa, nearly 2.52 times that of the pure membrane. The proton conductivity of the 1Me@GO/ABPBI composite membrane reached 0.01 S cm-1 across a wide temperature range (40-180 °C), peaking at 0.087 S cm-1 at 180 °C. Additionally, a single-cell incorporating the 1Me@GO/ABPBI composite membrane achieved a peak power density of 0.304 W cm-2 at 160 °C, nearly 1.46 times that of the pure membrane. Benefiting from the well-dispersed and PA-enriched proton channels provided by Me@GO, the Me@GO/ABPBI composite membrane exhibits excellent prospects for wide-temperature range (40-180 °C) applications.

4.
ACS Nano ; 18(40): 27358-27371, 2024 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-39313911

RESUMO

Air-rechargeable batteries integrating energy harvesting, conversion, and storage provide the most portable and popular approach to self-charging power systems. However, air-rechargeable batteries are currently mostly aqueous Zn-based battery systems in which it has remained a significant challenge to solve the low discharge capacities and poor cycling stability of chemical self-charging due to continuous insertion/extraction of large-size hydrated Zn2+. Herein, efficient Bi2Te3@C cathodes with an active carbon paper substrate are developed. Further ex situ characterization analysis confirms the energy storage mechanism regarding the coexistence of H+/Zn2+ coinsertion and conversion reaction in the aqueous Zn||Bi2Te3@C battery. Benefiting from the fast dynamics process attributed to the unique mechanism, a reliable energy supply is provided even in an extended temperature range from -10 to 45 °C. More importantly, Bi2Te3@C cathodes boost the superior and repeatable air-rechargeability. A discharge capacity of up to 264.20 mA h g-1 at 0.30 A g-1 is manifested after self-charging for 11.00 h. In addition, two quasi-solid-state battery devices are connected in series to continuously power a timer. After the device is discharged and then air self-charged for just a few seconds, an LED is lit.

5.
Small ; : e2405643, 2024 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-39308314

RESUMO

Aqueous flow batteries (AFBs) are promising long-duration energy storage system owing to intrinsic safety, inherent scalability, and ultralong cycle life. However, due to the thicker (3-5 mm) and heavier (300-600 g m-2) nature, the current used graphite felt (GF) electrodes still limit the volume/weight power density of AFBs. Herein, a lightweight (≈50 g m-2) and ultrathin (≈0.3 mm) carbon microtube electrode (CME) is proposed derived from a scalable one-step carbonization of commercial cotton cloth. The unique loose woven structure composed of carbon microtube endows CME with excellent conductivity, abundant active sites, and enhanced electrolyte transport performance, thereby significantly reducing polarization in working AFBs. As a consequence, CME demonstrates excellent cycling performance in pH-universal AFBs, including acidic vanadium flow battery (maximum power density of 632.2 mW cm-2), neutral Zn-I2 flow battery (750 cycles with average Coulombic efficiency of 99.6%), and alkaline Zn-Fe flow battery (energy efficiency over 70% at 200 mA cm-2). More importantly, the estimated price of CME is only 5% of GF (≈3 vs ≈60 $ m-2). Therefore, it is reasonably anticipated that the lightweight and ultrathin CME may emerge as the next generation electrode for AFBs.

6.
Adv Mater ; 36(38): e2406343, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39096067

RESUMO

To improve the performance of Lithium-Sulfur (Li-S) batteries, the reaction catalysts of lithium polysulfides (LiPSs) reactions should have the characteristics of large surface area, efficient atomic utilization, high conductivity, small size, good stability, and strong adjustability. Herein, Anderson-type polyoxometalate ([TMMo6O24]n-, TM = Co, Ni, Fe, represented by TMMo6 POMs) are used as the modified materials for Li-S battery separator. By customizing the central metal atoms, this work gains insights into the layer-by-layer electron transfer mechanism between TMMo6 units and LiPSs, similar to the collision effect of a bowling ball. Theoretical analysis and in situ experimental characterization show that the changes of CoMo6 units with moderate binding energy and lowest Gibbs free energy result in the formation of robust polar bonds and prolonged S─S bonds after adsorption. Hence, the representative Li-S battery with CoMo6 and graphene composite modified separator has a high initial capacity of 1588.6 mA h g-1 at 0.2 C, excellent cycle performance of more than 3000 cycles at 5 C, and uniform Li+ transport over 1900 h. More importantly, this work has revealed the inherent contradiction between the kinetics and thermodynamics, achieving a stable cycle in the temperature range of -20 to 60 °C.

7.
Adv Mater ; 36(39): e2406135, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38869350

RESUMO

Wide operation temperature is the crucial objective for an energy storage system that can be applied under harsh environmental conditions. For lithium-sulfur batteries, the "shuttle effect" of polysulfide intermediates will aggravate with the temperature increasing, while the reaction kinetics decreases sharply as the temperature decreasing. In particular, sulfur reaction mechanism at low temperatures seems to be quite different from that at room temperature. Here, through in situ Raman and electrochemical impedance spectroscopy studies, the newly emerged platform at cryogenic temperature corresponds to the reduction process of Li2S8 to Li2S4, which will be another rate-determining step of sulfur conversion reaction, in addition to the solid-phase conversion process of Li2S4 to Li2S2/Li2S at low temperatures. Porous bismuth vanadate (BiVO4) spheres are designed as sulfur host material, which achieve the rapid snap-transfer-catalytic process by shortening lithium-ion transport pathway and accelerating the targeted rate-determining steps. Such promoting effect greatly inhibits severe "shuttle effect" at high temperatures and simultaneously improves sulfur conversion efficiency in the cryogenic environment. The cell with the porous BiVO4 spheres as the host exhibits excellent rate capability and cycle performance under wide working temperatures.

8.
Adv Mater ; 36(32): e2405473, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38837833

RESUMO

In the pursuit of high-performance energy storage systems, four-electron zinc-iodine aqueous batteries (4eZIBs) with successive I-/I2/I+ redox couples are appealing for their potential to deliver high energy density and resource abundance. However, susceptibility of positive valence I+ to hydrolysis and instability of Zn plating/stripping in conventional aqueous electrolyte pose significant challenges. In response, polyethylene glycol (PEG 200) is introduced as co-solvent in 2 m ZnCl2 aqueous solution to design a wide temperature electrolyte. Through a comprehensive investigation combining spectroscopic characterizations and theoretical simulations, it is elucidated that PEG disrupts the intrinsic strong H-bonds of water by global weak PEG-H2O interaction, which strengthens the O─H covalent bond of water and intensifies the coordination with Zn2+. This synergistic effect substantially reduces water activity to restrain the I+ hydrolysis, facilitating I-/I2/I+ redox kinetics, mitigating I3 - formation and smoothening Zn deposition. The 4eZIBs in the optimized hybrid electrolyte not only deliver superior cyclability with a low fading rate of 0.0009% per cycle over 20 000 cycles and a close-to-unit coulombic efficiency but also exhibit stable performance in a wide temperature range from 40 °C to -40 °C. This study offers valuable insights into the rational design of electrolytes for 4eZIBs.

9.
Angew Chem Int Ed Engl ; 63(34): e202407303, 2024 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-38837854

RESUMO

The Li-CO2 batteries utilizing greenhouse gas CO2 possess advantages of high energy density and environmental friendliness. However, these batteries following Li2CO3-product route typically exhibit low work voltage (<2.5 V) and energy efficiency. Herein, we have demonstrated for the first time that cobalt phthalocyanine (CoPc) as homogeneous catalyst can elevate the work plateau towards 2.98 V, which is higher than its theoretical discharge voltage without changing the Li2CO3-product route. This unprecedented discharge voltage is illustrated by mass spectrum and electrochemical analyses that CoPc has powerful adsorption capability with CO2 (-7.484 kJ mol-1) and forms discharge intermediate of C33H16CoN8O2. Besides high discharge capacity of 18724 mAh g-1 and robust cyclability over 1600 hours (1000 mAh g-1 cut-off) at a current density of 100 mA g-1, the batteries show high temperature adaptability (-30-80 °C). Our work is paving a promising avenue for the progress of high-efficiency Li-CO2 batteries.

10.
ACS Nano ; 18(20): 12981-12993, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38717035

RESUMO

Aqueous aluminum-ion batteries (AAIBs) are considered as a promising alternative to lithium-ion batteries due to their large theoretical capacity, high safety, and low cost. However, the uneven deposition, hydrogen evolution reaction (HER), and corrosion during cycling impede the development of AAIBs, especially under a harsh environment. Here, a hydrated eutectic electrolyte (AATH40) composed of Al(OTf)3, acetonitrile (AN), triethyl phosphate (TEP), and H2O was designed to improve the electrochemical performance of AAIBs in a wide temperature range. The combination of molecular dynamics simulations and spectroscopy analysis reveals that AATH40 has a less-water-solvated structure [Al(AN)2(TEP)(OTf)2(H2O)]3+, which effectively inhibits side reactions, decreases the freezing point, and extends the electrochemical window of the electrolyte. Furthermore, the formation of a solid electrolyte interface, which effectively inhibits HER and corrosion, has been demonstrated by X-ray photoelectron spectroscopy, X-ray diffraction tests, and in situ differential electrochemical mass spectrometry. Additionally, operando synchrotron Fourier transform infrared spectroscopy and electrochemical quartz crystal microbalance with dissipation monitoring reveal a three-electron storage mechanism for the Al//polyaniline full cells. Consequently, AAIBs with this electrolyte exhibit improved cycling stability within the temperature range of -10-50 °C. This present study introduces a promising methodology for designing electrolytes suitable for low-cost, safe, and stable AAIBs over a wide temperature range.

11.
ACS Nano ; 18(16): 10863-10873, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38613506

RESUMO

A Na4MnV(PO4)3 (NMVP) cathode is regarded as a promising cathode candidate for sodium-ion batteries (SIBs). However, issues such as low electronic conductivity and partial cation dissolution contribute to high polarization and structure distortion. Herein, we engineered the local electron density and reaction kinetic properties of NMVP cathodes with varying oxygen vacancies by introducing varying amounts of Zr doping and carbon coating. The optimized sample exhibited a high-rate capacity of 71.8 mAh g-1 at 30 C (83.1% capacity retention after 1000 cycles) and excellent performance over a wide temperature range (84.1 mAh g-1 at 60 °C and 61.4 mAh g-1 at -30 °C). In situ X-ray diffraction technology confirmed a redox solid solution and a two-phase reaction mechanism, revealing minor changes in cell volume and slight strain variations after Zr doping, effectively suppressing the structural distortion. Theoretical calculations illustrated that Zr doping largely shrinks the band gap of NMVP, enriches local electron density, and slightly alters the local element distribution and bond lengths. Moreover, full-cells have shown high energy density (259.9 Wh kg-1) and outstanding cycling stability (200 cycles). The work provides fresh insights into the synergistic effect of strain suppressing and interface engineering in promoting the development of wide temperature range and long-calendar-life SIBs.

12.
Small ; 20(33): e2400980, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38545991

RESUMO

Polyolefin separators are the most commonly used separators for lithium batteries; however, they tend to shrink when heated, and their Li+ transference number (t Li +) is low. Metal-organic frameworks (MOFs) are expected to solve the above problems due to their high thermal stability, abundant pore structure, and open metal sites. However, it is difficult to prepare high-porosity MOF-based membranes by conventional membrane preparation methods. In this study, a high-porosity free-standing MOF-based safety separator, denoted the BCM separator, is prepared through a nano-interfacial supramolecular adhesion strategy. The BCM separator has a large specific surface area (450.22 m2 g-1) and porosity (62.0%), a high electrolyte uptake (475 wt%), and can maintain its morphology at 200 °C. The ionic conductivity and t Li + of the BCM separator are 1.97 and 0.72 mS cm-1, respectively. Li//LiFePO4 cells with BCM separators have a capacity retention rate of 95.07% after 1100 cycles at 5  C, a stable high-temperature cycling performance of 300 cycles at 80 °C, and good capacity retention at -40 °C. Li//NCM811 cells with BCM separators exhibit significantly improved rate performance and cycling performance. Pouch cells with BCM separators can work at 120 °C and have good safety at high temperature.

13.
Small ; 20(30): e2312116, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38446107

RESUMO

Flexible zinc-ion batteries have garnered significant attention in the realm of wearable technology. However, the instability of hydrogel electrolytes in a wide-temperature range and uncontrollable side reactions of the Zn electrode have become the main problems for practical applications. Herein, N,N-dimethylformamide (DMF) to design a binary solvent (H2O-DMF) is introduced and combined it with polyacrylamide (PAM) and ZnSO4 to synthesize a hydrogel electrolyte (denoted as PZD). The synergistic effect of DMF and PAM not only guides Zn2+ deposition on Zn(002) crystal plane and isolates H2O from the Zn anode, but also breaks the hydrogen bonding network between water to improve the wide-temperature range stability of hydrogel electrolytes. Consequently, the symmetric cell utilizing PZD can stably cycle over 5600 h at 0.5 mA cm- 2@0.5 mAh cm-2. Furthermore, the Zn//PZD//MnO2 full cell exhibits favorable wide-temperature range adaptability (for 16000 cycles at 3 A g-1 under 25 °C, 750 cycles with 98 mAh g-1 at 0.1 A g-1 under -20 °C) and outstanding mechanical properties (for lighting up the LEDs under conditions of pressure, bending, cutting, and puncture). This work proposes a useful modification for designing a high-performance hydrogel electrolyte, which provides a reference for investigating the practical flexible aqueous batteries.

14.
Angew Chem Int Ed Engl ; 63(23): e202317923, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38536212

RESUMO

Lithium metal battery has been regarded as promising next-generation battery system aiming for higher energy density. However, the lithium metal anode suffers severe side-reaction and dendrite issues. Its electrochemical performance is significantly dependant on the electrolyte components and solvation structure. Herein, a series of fluorinated ethers are synthesized with weak-solvation ability owing to the duple steric effect derived from the designed longer carbon chain and methine group. The electrolyte solvation structure rich in AGGs (97.96 %) enables remarkable CE of 99.71 % (25 °C) as well as high CE of 98.56 % even at -20 °C. Moreover, the lithium-sulfur battery exhibits excellent performance in a wide temperature range (-20 to 50 °C) ascribed to the modified interphase rich in LiF/LiO2. Furthermore, the pouch cell delivers superior energy density of 344.4 Wh kg-1 and maintains 80 % capacity retention after 50 cycles. The novel solvent design via molecule chemistry provides alternative strategy to adjust solvation structure and thus favors high-energy density lithium metal batteries.

15.
ACS Nano ; 18(6): 5132-5140, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38311845

RESUMO

Flexible all-solid-state lithium-carbon dioxide batteries (FASSLCBs) are recognized as a next-generation energy storage technology by solving safety and shuttle effect problems. However, the present FASSLCBs rely heavily on high-temperature operation due to sluggish solid-solid-gas multiphase mass transfer and unclear capacity degradation mechanism. Herein, we designed bicontinuous hierarchical porous structures (BCHPSs) for both solid polymer electrolyte and cathode for FASSLCBs to facilitate the mass transfer in all connected directions. The formed large Lewis acidic surface effectively promotes the lithium salt dissociation and the CO2 conversion. Furthermore, it is unraveled that the battery capacity degradation originates from the "dead Li2CO3" formation, which is inhibited by the fast decomposition of Li2CO3. Accordingly, the assembled FASSLCBs exhibit an excellent cycling stability of 133 cycles at 60 °C, which is 2.7 times longer than that without BCHPSs, and the FASSLCBs can be operated repeatedly even at room temperature. This BCHPS method and fundamental deactivation mechanism provide a perspective for designing FASSLCBs with long cycling life.

16.
ACS Appl Mater Interfaces ; 16(10): 12821-12832, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38416064

RESUMO

Next-generation high-temperature applications increasingly rely heavily on advanced thermistor materials with enhanced thermal stability and electrical performance. However, thus far, the great challenge of realizing high thermal stability and precision in a wide temperature range has become a key bottleneck restricting the high-temperature application. Here, we propose a high-entropy strategy to design novel high-temperature thermistor ceramics (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)NbO4. Differences in atomic size, mass, and electronegativity in this high-entropy system cause high lattice distortion, substantial grain boundaries, and high dislocation density. These enhance the charge carrier transport and reduce the grain boundary resistance, thus synergistically broadening the temperature range. Our samples maintain high precision and thermal stability over a wide temperature range from room temperature to 1523 K (ΔT = 1250 K) with an aging value as low as 0.42% after 1000 h at 1173 K, showing breakthrough progress in high-temperature thermistor ceramics. This study establishes an effective approach to enhancing the performance of high-temperature thermistor materials through high-entropy strategies.

17.
Nano Lett ; 24(5): 1729-1737, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38289279

RESUMO

Rechargeable hydrogen gas batteries, driven by hydrogen evolution and oxidation reactions (HER/HOR), are emerging grid-scale energy storage technologies owing to their low cost and superb cycle life. However, compared with aqueous electrolytes, the HER/HOR activities in nonaqueous electrolytes have rarely been studied. Here, for the first time, we develop a nonaqueous proton electrolyte (NAPE) for a high-performance hydrogen gas-proton battery for all-climate energy storage applications. The advanced nonaqueous hydrogen gas-proton battery (NAHPB) assembled with a representative V2(PO4)3 cathode and H2 anode in a NAPE exhibits a high discharge capacity of 165 mAh g-1 at 1 C at room temperature. It also efficiently operates under all-climate conditions (from -30 to +70 °C) with an excellent electrochemical performance. Our findings offer a new direction for designing nonaqueous proton batteries in a wide temperature range.

18.
Angew Chem Int Ed Engl ; 63(10): e202318204, 2024 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-38244210

RESUMO

Aluminum-sulfur (Al-S) batteries are promising energy storage devices due to their high theoretical capacity, low cost, and high safety. However, the high viscosity and inferior ion transport of conventionally used ionic liquid electrolytes (ILEs) limit the kinetics of Al-S batteries, especially at sub-zero temperatures. Herein, locally concentrated ionic liquid electrolytes (LCILE) formed via diluting the ILEs with non-solvating 1,2-difluorobenzene (dFBn) co-solvent are proposed for wide-temperature-range Al-S batteries. The addition of dFBn effectively promotes the fluidity and ionic conductivity without affecting the AlCl4 - /Al2 Cl7 - equilibrium, which preserves the reversible stripping/plating of aluminum and further promotes the overall kinetics of Al-S batteries. As a result, Al-S cells employing the LCILE exhibit higher specific capacity, better cyclability, and lower polarization with respect to the neat ILE in a wide temperature range from -20 to 40 °C. For instance, Al-S batteries employing the LCILE sustain a remarkable capacity of 507 mAh g-1 after 300 cycles at 20 °C, while only 229 mAh g-1 is delivered with the dFBn-free electrolyte under the same condition. This work demonstrates the favorable use of LCILEs for wide-temperature Al-S batteries.

19.
Adv Mater ; 36(11): e2310623, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38088907

RESUMO

The practical implementation of aqueous zinc-ion batteries (AZIBs) encounters challenges such as dendrite growth, parasitic reactions, and severe decay in battery performance under harsh environments. Here, a novel hydrated eutectic electrolyte (HEE) composed of Zn(ClO4 )2 ·6H2 O, ethylene glycol (EG), and InCl3 solution is introduced to effectively extend the lifespan of AZIBs over a wide temperature range from -50 to 50 °C. Molecular dynamics simulations and spectroscopy analysis demonstrate that the H2 O molecules are confined within the liquid eutectic network through dual-interaction, involving coordination with Zn2+ and hydrogen bonding with EG, thus weakening the activity of free water and extending the electrochemical window. Importantly, cryo-transmission electron microscopy and spectroscopy techniques reveal that HEE in situ forms a zincophobic/zincophilic bilayer interphase by the dissociation-reduction of eutectic molecules. Specifically, the zincophilic interphase reduces the energy barrier for Zn nucleation, promoting uniform Zn deposition, while the zincophobic interphase prevents active water from contacting the Zn surface, thus inhibiting the side reactions. Furthermore, the relationships between the structural evolution of the liquid eutectic network and interfacial chemistry at electrode/electrolyte interphase are further discussed in this work. The scalability of this design strategy can bring benefits to AZIBs operating over a wide temperature range.

20.
Small ; 20(24): e2310992, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38155518

RESUMO

With the rapid development and increasing popularity of electric vehicles and wearables, battery safety has become a leading focus in the field of energy storage research. Specifically, aluminum-ion batteries are gaining increasing attention as low-cost energy-storage systems with high safety levels and theoretical energy density. However, the dense alumina passivation layer on the aluminum anode surface and slow kinetic performance of commonly used ionic liquid electrolytes still render poor performance. This report presents a new type of aluminum-derived lithium-ion battery (ALIB) that maintains a certain discharge performance under damaging conditions, including continuous bending, high- and low-temperature environments, and shearing. This new ALIB effectively meets the current demand for flexible and wearable batteries. The prepared ALIB achieves a stable cycle of 130 mAh g-1 specific capacity and ≈260 Wh kg-1 theoretical energy density at a wide voltage platform of 2 V and a test temperature of 25 °C without undergoing combustion. Additionally, the study analyzes the reaction mechanism of this ALIB based on density functional theory and conducts ex situ XRD and XPS analyses to elucidate the underlying storage mechanism.

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